Documente Academic
Documente Profesional
Documente Cultură
ENVIRONMENTAL POLLUTION
VOLUME 4
Editors
Brian J. Alloway, Department (}fSoil Science, The University ofReading, UK.
Jack T Trevors, Department (~fEnvironmental Biolo!?y, University (~f Guelph, Ontario,
Canada
Editorial Board
T Anderson, The Institute ()(Environmental and Human Health, Texas Tech University,
Lubbock, Us.A.
TH. Christensen, Department (~!"Environmental Science and Engineering, Danislt
Tecltnical University, Lyngby, Denmark
I. Colbeck, Institutelor Environmental Research, Department ()!" Biolo!?ical Sciences,
University ()f Essex, Colcltester, UK.
K.c. Jones, Institute ()!" Environmental and Natural Sciences, Lancaster Universi(v, u.K.
S. Parry, TH. Huxley Scltool (~!" Environment, Earth Sciences and Engineering, Imperial
College at Silwood Park, Ascot, Berks, u.K.
W. Salomons, GKSS Research Center, Geesthacht, Gennany
Bioreactors for
Waste Gas Treatment
edited by
C. Kennes
and
M.C. Veiga
University (~t"La Comiia,
La CoruFia, Spain
Preface Xlll
Acknowledgments xv
Contributors XVll
• PART 1 PRINCIPLES 1
References 298
Chapter 14 Odour control at waste water treatment plants by diffusion
into activated sludge basins 299
1. Introduction 299
2. Summary ofreported problems 299
2.1. Corrosion 299
2.2. Organic film accumulation 299
3. Concord, New Hampshire, case study 303
4. Valley Forge, Pennsylvania, case study 303
5. Annapolis, Maryland, case study 305
Index 307
Preface X11l
PREFACE
Air pollution is, and will certainly remain, one of the major problems to be solved
over the next century. Severa! conventional physical and chemical technologies have
been deve10ped and set up over the past decades, and many books describing such
techniques have been published. However, more recently new treatment alternatives
have been tested, based on the use of bioreactors. It very quickly appeared that such
systems present several advantages, among which are their high efficiency and low
cost. The treatment of polluted air in bioreactors allows the complete destruction of
the contaminants, contrary to such conventional technologies as adsorption or
absorption transferring the contaminant from one phase (gas) to another (liquid or
solid). In bioreactors pollutants are oxidised by microorganisms into innocuous
products. In more c1assical technologies, such as thermal or catalytic incineration,
pollutants are oxidised as well, but usually at rather higher investment and operation
costs.
An ever increasing number of research studies related to biological waste gas
treatment in bioreactors have been published in scientific journals, as well as some
review papers mainly on conventional biofilters. The conventional biofilter
represents the first developed reactor design for air pollution control. A large number
of such bioreactors have been installed relative1y recently, in Europe, Canada and the
United States, as well as in many other developed countries. Most of those reactors
operate successfully for solving air pollution problems. Over the past decade the
efficiency of biofilters has been improved further and the application fields have
been broadened. New bioreactor designs have been studied, as well. Biotrickling
filters (or trickling biofilters) and bioscrubbers are two such new designs that were
first studied at lab-scale. Full-scale systems were installed later, many of which have
now been operating successfully for several years in the field. The same holds true
for systems such as Rotating Biological Contactors (RBC) and airlift bioreactors,
which are being used at industrial scale, though in a much more limited range of
applications. Odour diffusion into activated sludge basins is another alternative
technology for air pollution control. Finally, the lab-scale efficiency of some
relatively new bioreactor designs, such as photobioreactors and membrane
bioreactors is at present actively being evaluated in research laboratories.
As bioreactors appear to be of great interest for solving air pollution
problems, no doubt a book on this topic was highly needed. This is the first book
presenting in a single volume a complete comprehensive overview of all major
bioreactor designs presently available on the market. A few chapters are also
dedicated to systems still at the lab-scale or pilot-scale research stage. A complete
chapter focuses on c1assical non-biological alternatives, allowing easy comparison of
physical, chemical and bioreactor technologies, and a more efficient selection of the
most suitable techniques for industrial-scale applications. The book is divided in two
parts. The first part is dedicated to explaining the principles of the different
techniques, while full-scale bioreactor applications are detailed for each system in
the second part of the book. Each chapter has been written by experts with much
experience in the specific bioreactor being described.
As different fundamental and applied aspects are presented, the book will be
of value to a broad range of potential readers in industry, environmental agencies, as
well as in academia. It will certainly be of interest to professors teaching graduate
XIV Preface
Christian Kennes
Maria C. Vciga
xv
ACKNOWLEDGMENTS
The editors would like to thank the many colleagues, students, researchers, friends,
and all people in general who helped to some extent preparing this book. Special
thanks are due to the students and technician that helped preparing some of the
Figures and that collaborated in offering suggestions and in revising the chapters. We
are grateful to the companies who provided information and illustrative material
which has enabled us to improve the quality of the manuscript. We would especially
like to acknowledge the collaboration of Tecnium, Plastoquimica and Kalfrisa.
We are indebted to the organisations that make our work on air pollution
control possible. These include regional (Xunta de Galicia), national (Ministry of
Science and Technology) and European organisations and funding agencies.
Last but not least, the editors would like to thank the contributing authors and
the Publisher for their efficient cooperation.
Contributors XVII
CONTRIBUTORS
Robert P.G. Bowker, Bowker and Associates Inc., 477 Congress Street, Suite 1004,
Portland, ME 04101. (Chapter 14)
Niels G. Hansen, Kriiger AlS, 363 Gladsaksevej, DK-2860 Soeborg (Chapter 13).
N.J.R. Kraakman, Bioway B.V., P.O Box 361, NL-6710 BJ Ede. (Chapter 12)
PhiIipp Rudolf von Rohr, ETH Centre, Institute of Process Engineering, CH-8092
Zurich. (Chapter 8).
1. The atmosphere
The atmosphere is a gas layer several hundreds of kilometres thick sUITounding the
earth. The average chemical composition of clean, dry atmospheric air is almost
constant, as presented in Table 1.1. In fact, atmospheric air also contains 1 to 3%
water vapour. Except for nitrogen and inert gases characterised by a basically
constant concentration and with an almost permanent residence rime, other
compounds listed in the table present a hmited residence time. The residence time of
compounds, such as ammonia, hydrogen sulphide or nitric oxide, is only a few days.
Although they are naturally present in the atmosphere, they may become
contaminants if their concentration increases, for extended periods of time, above
trace levels or above concentrations listed in Table 1.1.
Alterations in the composition of clean atmospheric air may originate from either
natural or anthropogenic sources. Natural sources have been present on earth for
ages, while pollution from anthropogenic sources appeared more recently and has
increased exponentially with the industrial revolution.
The intensity of natural pollution depends on many factors, such as location,
vegetation and temperature. Among the main natural sources of pollutants are
volcanic eruptions. Volcanoes are major sources of particlcs and ash, volatile
hydrocarbons, sulphur dioxide and hydrogen sulphide, the latler being oxidised to
S02 in the atmosphere. Among other natural sources are forest fires that may
produce smoke, ash and volatile gases. Decay of organic matler is a source of
ammonia, nitrous oxide (N20) aud methane, among others. It is interesting to note
that on an annual basis, some contaminants, such as hydrogen sulphide, some
nitrogen compounds, hydrocarbons, carbon monoxide, etc., are produced to a larger
extent from natural sources than from non-natural ones. However, anthropogenic
sources may be more harmful, since contaminant release may often be more
intensive locally and for prolonged periods of time. They are, in most cases, located
near regions with high population densities.
Anthropogenic sources are related to human and industrial activities. They
can be classified into stationary sources and mobile sources. Stationary sources
include domestic sources, mainly heating devices, and industrial sources releasing
contaminants largely through combustion processes and via ali kinds of waste gases
in general. Waste gases released from waste water treatment plants, composting or
other waste treatment processes are considered stationary sources, as well. Air
pollution may also result from remediation technologies transferring volatile or semi-
volatile contaminants from soil or aquifers into the atmosphere. Anthropogenic
mobile sources refer to ali types of vehicles, aeroplanes, boats and any other kind of
transportation related source.
Bioreactor technologies described in this book are, at this stage, only applied
to stationary sources. Such technologies are only suitable for the removal of
vapours/odours, and particulate matter often needs to be removed by other non-
biological processes first, to avoid problems during the biological treatment.
Treatment of VOCs from industrial waste gases is a relatively new application of
bioreactor technologies. Conversely, the treatment of odours from some specific
sources using conventional biofilters has been applied for several decades. especially
in the case of air pollution problems related to waste water treatment plants and
composting facilities (Chapter 3).
For some pollutants, their release from motor vehicle engines, as a result of
inefficient combustion of fuel, is much more important than the release from
industrial or domestic sources. This is particularly true for carbon monoxide and
some specific hydrocarbons. Vehicle combusters are usually optimi sed to achieve
maximal power aud performance, rather than for minimising pollution. Major
compounds released from vehicles are water vapour, nitrogen oxides (NOx), carbon
dioxide, carbon monoxide, sulphur dioxide, hydrocarbons, particles and lead. Water
vapour and carbon dioxide are usually not considered to be contaminants. Several
Fundamentals 5
methods have been adopted to reduce air pollution from mobile sources, mainly cars
and trucks. Emissions of carbon monoxide, nitrogen oxides and hydrocarbons have
been reduced over the past decades by using catalysts in so called catalytic
converters. Exhaust gas recirculation is another way to decrease emissions of
nitrogen oxides. Since lead is a contaminant and does also poison catalysts, its
concentration has been drastically reduced in gasoline, reducing at the same time, air
contamination by lead. It does, however, affect fuel octane number which can be
compensated for by adding oxygenates to gasoline as methyl-ter-butyl-ether (MTBE)
or ethyl-ter-butyl-ether (ETBE). This does also allow reduction, to some extent, of
carbon monoxide and VOC emissions, at least at high engine loading (Osman et al.,
1993, Poulopoulos and Philippopoulos, 2000). Nevertheless, MTBE and ETBE are
aIso toxic and have been detected in the exhaust gas of vehic1es. The automotive
industry continues searching for alternative ways of reducing air contamination.
related products, such as gasoline, might appear as a potential problem for biological
treatment. However, gasoline mainly composed of alkylbenzenes and alkanes is
biodegradable by many microorganisms when the VOCs are present at relatively low
concentrations (Hodge et al., 1991; Mikesell et al., 1993; Kennes et al., 1996).
2.2.6. Composting
Composting is a fermentation process used for (bio )degrading the organic fraction of
organic waste into a stable humus-like product. Many different substrates have been
used for composting: waste water sludge, yard waste, forest sub-products, bark, etc.
As in basically ali fermentation processes the prime matter is degraded into smaller
volatile products. Odour problems are often linked to composting. Although
fermentation usually takes place under aerobic conditions, anaerobic zones may
sometimes also appear in composting piles resulting in the release of highly odorous
metabolites. Unbalanced C:N ratios are also favourable to the formation and
volatilisation of odorous compounds, such as ammonia formed in the presence of
excess nitrogen. Other volatile compounds typically formed during composting
include sulphides, mercaptans, amines, fatty acids (typical of anaerobic
biodegradation), ketones and some aromatic compounds (Derikx et al., 1989; Hentz
et al., 1992; Miller et al., 1991; Prokop and Bohn, 1985). Treatment of composting
odours is one ofthe original applications ofbiofiltration (Prokop and Bohn, 1985).
Fundamentals 7
Table 1.2. Waste gases and air pollution problems treated with bioreactors
The most easily detectable air pollutants are those related to smell or odour
problems. Other contaminants leading to air pollution problems, such as carcinogenic
compounds, are sometimes more difficult to detect, though they are not less harmful.
Their effect is often visible only after several years. This is also the case of, for
example, acid rain affecting monurnents, since the degradation process is only
detectable after quite a long period of exposure. The most important air pollutants
are, on the one hand, partic1es, and on the other hand, gases or vapours comprising
volatile organic compounds (VOCs), volatile inorganic compounds (VICs) and
odours. Although both VOCs and VICs may contribute to odour problems, we will
detine and explain odour problems separate1y.
3.1 PARTICLES
Particulate matter refers to either solid or liquid dispersed matter present in the air
and larger than 0.0002 Ilm -the mean size of single small molecules- but smaller
than about 500 Ilm (Wark and Wamer, 1989). Different types of partic1es may be
considered. Aerosols and partic1es represent virtually the same concept, though the
former is slightly more restrictive, since aerosols refer to all liquid or solid airbome
suspensions generally smaller than 1 Ilm. Dust and fumes are solids. Dust results
from grinding or crushing operations and fumes re suit from vapour condensation.
Liquid partic1es are often called mist or fog. Smoke is another type of particu1ate
matter re1eased from incomplete combustion processes. Soot is carbon particles also
10 C. Kennes and MC. Veiga
re1eased during combustion processes. In 1973, it was estimated that about 9% of the
total mass of air contaminants were partic1es. This value has slightly decreased over
the last decades. Particles are released both from mobile sources and from stationary
sources. Some particles may carry substances, such as carcinogenic organic
compounds. Particles cannot be removed in biological reactors. They need to be
removed in a pre-treatment step, should waste gases containing both particles and
volatile pollutants need to be treated in bioreactors. Possible pre-treatment processes
for the removal of particulate matter include filters, cyc1ones, electrostatic
precipitators, etc., as described in Chapter 2.
Different definitions have been proposed for the different forms in which gases or
vapours may be found in polluted air. Definitions may vary depending on the
country, region or state. Using the temperature as reference, VOCs are organic
chemicals (vapours) containing carbon atoms and which have a normal boi ling
temperature be10w 100 aC, at 101 kPa. In some cases, a higher maximal normal
boiling temperature of 260 °c is mentioned. If one uses pressure as the key
parameter, VOCs are pollutants with a vapour pressure greater than 0.014 kPa at 25
aC. Here again other definitions can be found and vapour pressures greater than 0.07
kPa are sometimes used for defining VOCs. In the United States, VOCs are
sometimes defined as any organic carbon compound, excluding carbon monoxide,
carbon dioxide, carbonic acid, metallic carbides and carbonates, and ammonium
carbonate, which partlclpates in atmospheric photochemical reactions.
Photochemical reactions are reactions initiated in the presence of solar radiation and
involving pollutants, such as VOCs, NO x and atmospheric oxygen. Free radicals are
then generated, initiating new reactions leading to environmental problems, such as,
among others, smog formation. VOCs include most hydrocarbons. Howcver,
methane is excluded from the list of hydrocarbons as it is relatively nonreactive.
Some other volatile compounds are not significantly involved in photolysis and
should also be excluded from the group of VOCs, such as ethane, acetone, t-
butylacetate, dichloromethane and several halogenated compounds, including many
CFCs, HFCs and HCFCs. When the gases or vapours are inorganic, they are called
Volatile Inorganic Compounds or VICs. Some examples of inorganic air pollutants
are sulphur dioxide, NO x, hydrogen sulphide, carbon disulphide, ammonia, etc ..
Once again it is interesting to note that several VOCs and VICs detected in the
atmosphere are emitted from biogenic sources.
Odour may be defined as a physiological stimulus of olfactory cells in the
presence of specific molecules. The nature and concentration of molecules detected
by olfactory cells varies between individuals and with environmental conditions,
such as temperature, pressure and humidity. According to the definition given above,
the terrn odour includes some VICs, as well as some VOCs. Odours may be very
unpleasant, as in the case of hydrogen sulphide and several other sulphur-
compounds. Other pollutants, such as esters, may seem pleasant initially, though they
often lead to major complaints when the odour problem remains for long periods of
time.
Many VICs as well as a relatively wide range of halogenated and non-
halogenated aromatic and aliphatic organic compounds (VOCs) are biodegradable by
microorganisms (van Agteren et al., 1998) and can be treated in bioreactors.
Fundamentals 11
4. Pollution quantification
where MW is the molecular weight ofthe contaminant and 24.5 or 22.4 represent the
volume occupied by one mole of an ideal gas at l atm and, respective1y, 25 °c or O
aC. From the above equations it can easily be concluded that for any temperature or
pressure the following equation applies:
(1.3)
4.20DOURS
In the case of odours, concentrations are commonly expressed in terms of odour units
per cubic meter or OU/m3 , allowing evaluation ofthe nuisance level to people living
in the surroundings of the odour producing source. One OU/m3 represents the
threshold amount of pollutant that will be detected by 50% of trained members of a
group, afler diluting the contaminant (odour) in one cubic meter of clean air under
standard conditions. This means that if, for a given pollutant, this minimal detectable
odour leve1 is, let us say, 100 ppmv, one OU/m3 ofthat compound will correspond to
100 ppmv. It can easily be understood that such a definition is less rigorous than
concentrations expressed in glm3 as mentioned previously for VOCs or VICs, since
the definition of an odour unit may vary depending on the persons included in the
group.
Another definition has recently been proposed by the European
Standardisation Committee. The European Odour Unit (European OUl m3) is defined
as the amount of pollutant (odour) that, diluted in one cubic meter of pure air under
standard conditions, leads to the same physiological response as a European
reference odour mass (EROM) diluted in one cubic meter of pure air under the same
conditions. One EROM is equivalent to 123 Ilg n-butanol.
12 C Kennes and MC Veiga
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Fundamentals 13
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Fundamentals 15
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CHAPTER 2 NON-BIOLOGICAL TREATMENT TECHNOLOGIES
1. Introduction
1
10 5 i
i
i INCINERATION :
i
i ,1
L._._._._._._._._._._._~_._._._._j
,,
: ABSORPTION
ADSORPTION ,,
,,,
~------------------
BIOREACTORS ,,
------------------~
(CRYO-)CONDENSAnON
o ~--------+---------~--------_+----------~--------~
10 10 2 103
Conccntration (glm 3)
Figure 2.1. Application range of major biological and non-biological air pollution control
technologies.
Several mature technologies are available on the market for the removal of
particulate matter. They wide1y differ in regards to costs and efficiencies. These
factors, together with the characteristics of the parti des to be removed, are the major
factors to be taken into account and to be compared, in order to se1ect the most
appropriate technology (Caputo and Pelagagge, 1999).
l7
C. Kennes and M. C. Veiga (eds.), Bioreactors for Waste Gas Treatment, 17-46.
© 2001 Kluwer Academic Publishers.
18 C Kennes el al.
4 g d p ( Pp - Pg ) (2.1 )
3 Pg C D
where
(2.2)
The numerical value of CD depends on the flow regime. In the laminar region
and turbulent region CD is basically constant and equal to (24/Re p) and 0.45,
respectively. Empirical equations are used for the transition region.
Assuming Pp » Pg, the theoretical collection efficiency (Il) representing the
fraction of partides that will be removed from the air stream can be calculated from:
7J
~)
= 1 - exp ( - V H
( g
= 1 - exp - 18
d/ PV HLJ
j1 g
p
(2.3)
where
L
~---------------------------------------------»
Air - - - .
inlet
, - - - . Treated
H:,, alf
,,,
2.2 CYCLONES
Although the collection mechanisms are to some extent similar to those in settling
chambers, in cyclones (Figure 2.3) a higher farce is applied on the particles than in
settling chambers. In inertial collectars ar cyclones. particulate matter is removed
from air by a centrifugal force. Its magnitude can be calculated from:
(2.4)
where
(2.5)
Treatcd air
Particlcs
2.3 FILTERS
(2.6)
Non-Biological Technologies 21
where
Subscripts f and c refer, respectively, to the fabric filter and to the cake.
2.3.2.1. Shakers. Dust laden air is usually flowing upwards through the bag (Figure
2.4). Particles are retained on the inside surface of the filter. Cleaning of the filter
consists of shaking the bags from the top, every few hours, allowing filtered particles
to fall into the hopper located beneath the baghouse. If continuous use of the shaker
is required, the collector needs to be compartmented in order to allow operation of a
portion of the collector to be stopped for cleaning while polluted air remains flowing
through the other portion ofthe baghouse (Cheremisinoff, 1993).
Treated air
Shaker
(or blower)
Filler
medium
. . . ţ . . . . . ţ .... ţ ..ţ . . ţ.
Air
inJet
J
Partieles
Figure 2.4. Shaker and Reverse flow cleaning system, equipped either with a shaking device
(in the case of a shaker) or with a blower (Reverse flow system) for cleaning the cloth.
22 C. Kennes et al.
2.3.2.2. Reverseflow cleaning. As in the case ofshakers, dust laden air is fed upflow
and particles accumulate upon the inner surface of the bag. Cleaning consists in
introducing clean air into the bags at low pressure and in the opposite direction to the
original flow of polluted air (Figure 2.4). As in the case of shakers, reverse flow
filters can be operated either in continuous mode by taking only few bags off line for
cleaning or they may be stopped temporarily for cleaning ofthe complete system.
2.3.2.3. Pu/se jet. In pul se jet collectors dust laden air flows inwards through the
bags. Particles accumulate on the outside surface of the filter. In order to maintain
their shape, the bags are held open by wire cages (Figure 2.5). A pulse of reverse
flow compressed air is passed through the filters, every few minutes, for cleaning the
cloth.
Blowpipe
Treateu _
+_ Compressed
air ţ:::~;:;::::==~===;;~==:::;:;:;-;==:=C mr
Rctainer
Filter
medium
t t t
Air
inlet
-J
Particles
Dischargc
electrode
~
Treated
~ air
Air~
inlel
~
Collecting
plate
Weight
The collection efficiency (ll) may be ca1culated with the Deutsch equation:
17 = 1 - exp
Vp A)
(-O (2.7)
where
Vp = migration velocity ofthe particle toward the collecting plate (m/s)
A = total area ofthe collecting plate (m2 )
Q = volumetric gas flow rate (m 3/s)
2.5 SCRUBBERS
Jlm, depending on the required efficiency and costs. Higher efficiencies are reached
when increasing the velocity of the fluids and decreasing droplet size. Different
designs are available. The most common ones are spray towers, cyclone scrubbers
and venturi scrubbers. However, scrubbers or absorption towers are best suited for
the removal of volatile compounds rather than for removing particles. Particulate
matter may lead to clogging problems. More data on absorption are also given in the
next section dealing with volatile compounds.
In spray towers, the solvent is introduced by means of a spray nozzle located
in the upper zone of the scrubber. Polluted air flows upwards and counter currently
(Figure 2.7). The particles may be captured by the water droplets through several
mechanisms, such as inertial impaction or diffusion. Other possible, though less
frequent, mechanisms include interception and electric attraction.
The collection efficiency of spray towers can be increased by increasing the
relative velocity between the water droplets and the air stream or particles in a
cyclone-scrubber, in which the velocity of the streams is increased by applying a
spinning motion to the fluids generating centrifugal forces. Such device is therefore
also suitable for slightly smaller particles than spray towers.
Trealed air
i
Waler ---. 0 - - - ' - - - - - - - - - 1 . - eli~~~lor
supply
Air ---.
inlel
Drain
water/sludge
3.1 ABSORPTION
In the case of absorption, contaminated air is put in contact with a non-volatile liquid
phase, the purpose being the mass transfer of the contaminant from the gas phase to
the liquid phase. Maximisation of the driving force and high diffusion rates are
requisites in order to reach an efficient separation. Solubility of the compound to be
transferred to the other phase and a high gas-liquid interfacial area will enhance the
process. In some cases, reaction between components ofthe gas phase and the liquid
phase may also take place (Shi el al., 1996; Thomas and Vanderschuren, 2000).
Often, the main disadvantage of this technique is that the pollutant is
transferred to a new phase instead of being destroyed, meaning that the pollution
problem remains present. However, such a characteristic becomes an advantage
whenever the contaminant is a relatively valuable chemical and when it needs to be
recovered for eventual resale or reuse.
Figure 2.8. Thr~c-pha s c absorptioll systelll pa~kcd with Rasehig rillgs IIsed for the treatillent
of odours from a waste water treatillent plant (Photo courtesy of Plastoquilllica).
parameter. Packings used in absorption towers are produced from various materials,
sizes and shapes. They may either be stacked in regular geometric patterns or
dumped at random. Some examples of common tower packings dumped at random
are PalI rings, Raschig rings, Hiflow rings and Intalox saddles made either of
ceramic, metal or plastic. The relative void fraction reached with such packings often
exceeds 0.8 or even 0.9. Honeycomb tubes as well as grids, sheets or spirals are
typical forms used in arranged packings.
3.1.2.2. Packed lowers. In packed towers (Figure 2.9) both phases flow in continuous
mode through the system reaching an intimate contact between the gas and the liquid
phase. The absorption tower is filled with a packing material characterised by its
high superficial area. The liquid phase flows through the column, reaching a large
gas- Iiquid superficial contact area thanks, among others, to the presence of the
packing material.
Counter-current, co-current or cross flows may be used, the first alternative
being the most popular one. In counter-current operation (Figure 2.1O-A) the liquid
phase is flowing downwards while the contaminated air is flowing counter-currently.
In such case a high relatively constant driving force is reached. Contrarily, in co-
current mode (Figure 2.10-8), the gas phase is put in contact with fresh liquid at the
entrance ofthe column. While passing through the absorption tower, the liquid phase
in contact with the contaminated air gets progressively more and more concentrated
in pollutant, with a concomitant decrease in the driving force . In case of cross flow
(Figure 2.1O-C), the gas phase flows horizontalIy while the liquid phase flows
vertically and downwards. Although less frequently used, this configuration does
sometimes present some advantages, such as a lower pressure drop and a lower
consumption of scrubbing liquid.
Non-Biological Technologies 27
Treated air
(G" y,)
Water inlet
~~~~*.- (L2. X2)
. - Airinlet
Water oudet .- r (G" y,)
(L"xl) --------'
t + ++
suppIy
~
PACKED PACKED PACKED Treated ~
COLUMN COLUMN ~ COLUMN air
iniet
t
Air
+
Drain Treated Drain
Drain
water
inlet water air water
A B c
Figure 2.10. Mode of operatiOl1 of absorption columns,
(2.8)
28 C Kennes el al.
where
Oi = Total molar flow rate of gas (air + pollutant) per unit cross sectional area of the
column (kmol/s.m2)
Li = Total molar flow rate ofliquid (water + pollutant) per unit cross sectional area of
the column (kmol/s.m2 )
Yi = mole fraction ofpollutant in the gas phase
Xi = mole fraction of pollutant in the liquid phase
Subscripts 1 and 2 refer, respectively, to the inlet and the outlet ofthe column for the
gas phase and to the outlet and the inlet ofthe liquid phase (Figure 2.9).
O and L vary along the height of the column, since there is a continuous mass
transfer of pollutants from one phase to the other. A mass balance equation with
constant molar flow rates can be written by modifying the above equation:
(2.9)
where
Os = molar flow rate of pollutant-free air per unit cross sectional area of column
(kmol/s.m2)
Ls = molar flow rate of pollutant-free liquid per unit cross sectional area of column
(kmol/s.m2)
Yi = moles ofpollutant per mole ofpollutant-free air in the gas phase
Xi = moles ofpollutant per mole ofpollutant-free liquid in the liquid phase
y, -y_l- (2.10)
1 - YI
~ (2.11)
Xi
1 - XI
Dropping the subscript 2 and solving for Y yields the equation of thc
operaling line valid both for packed towers and plate columns:
Y = Y - h (X - X) (2.12)
I Os I
Os dY = Ls dX (2.13 )
The equation of the rate of mass transfer of the pollutant from one phase to
another (Figure 2.11) is:
(2.14)
Non-Biological Technologies 29
or (2.15)
where
N A = molar flux of pollutant per unit time and area (kmolls.m 2)
k G (or ky) = individual gas phase mass transfer coefficient (kmolls.m 2 L'1p units of
concentration)
h (or k x) = individualliquid phase mass transfer coefficient (kmol/s.m 2 .L'lC units of
concentration)
PG (or YG) = partial pressure (or mole fraction) ofpollutant in the bulk gas phase
Pi (or Yi) = partial pressure (or mole fraction) ofpollutant at the interface
C L or XL = pollutant concentration (or mole fraction) in the bulk liquid
Ci or Xi = pollutant concentration (or mole fraction) at the interface
As the concentrations (i.e., Pi or Ci) and mole fractions (i.e., Yi and Xi) at the
interface level are usually hard to estimate, it is more convenient to use equilibrium
concentrations and overall mass transfer coefficients. The latter are obtained
experimentall y.
where
KG or Ky = overall mass transfer coefficient for the gas phase (kmolls.m 2 .L'lp units of
concentration)
Mass transfer, N A
Interface
Figure 2.11. Concentration profiles ofpollutant A in the gas phase and in the liquid phase.
30 C. Kennes el al.
K L or Kx = overall mass transfer eoeffieient for the liquid phase (kmol/s.m 2 6C units
of eoneentration)
p* = partial pressure of pollutant in equilibrium with the liquid phase eoneentration
CL
C* = pollutant eoneentration in equilibrium with pressure po in the gas phase
y* = equilibrium mole fraetion referred to the gas phase
x* = equilibrium mole fraetion referred to the liquid phase
The relationship between individual and overall mass transfer eoeffieients ean
easily by shown by eombining the above equations,
Kx kx
+
[:y (;: ~ :J] k,
+
mk y
(2.18)
and
Ky ky
+ [ ~k, ( y~ ~ y)]
XL XI
=
ky
+
m
k,
(2.19)
N A dA = Ky (y - y*) dA (2.20)
in whieh subseript G has been deleted from the parameter Yo for simplifying the
expression.
The mass transfer area (dA) is usually not known and ean advantageously be
substituted for another parameter (a) representing the interfaeial area per unit volume
of eolumn. Then, if S is the eross-seetional area of the tower,
dA=aSdz (2.21 )
and
N A a S dz = Ky a (y - y*) S dz (2.22)
The height of the eolumn ean be ealculated by eombining the mass balanee
equation and the mass transfer rate equation:
- G dy = Ky a (y - y*) S dz (2.23)
Non-Biological Technologies 31
Whenever relatively low pollutant concentrations are present in the gas phase,
(O/K y a S) will basically be constant and the total height (Z) of the system can be
estimated according to:
(2.24)
calling HTU the height of one transfer unit and NTU the total number of transfer
units needed for reaching the transfer of a given amount of pollutant from the gas
phase to the liquid phase.
(2.26)
with
(1 - y') - CI - y) (2.28)
(1 - y)lm
1-Y'
In (- -)
1 - Y
3.1.2.3. Plate columns. In plate columns (Figure 2.12) the phases flow in opposite
directions and the contact is intermittent. The liquid flows downwards from one plate
to another. Different plate designs are available. Each plate or stage allows an
intimate contact between the liquid and the gas phase, leading to diffusion and mass
transfer of the contaminant prior to phase separation. Calculation of the number of
theoretical equilibrium stages is an important design parameter which depends,
basically, on the composition of each phase and on equilibrium data. Since
equilibrium is not yet reached when both phases leave a given plate, the actual
number of stages should, afterwards, be estimated on the basis of a parameter known
as efficiency. Another design parameter is the column diameter. which is strongly
dependant on liquid and gas flows.
32 C. Kennes el al.
Clean
air outlet
i
..rf--------- Liquid in
1- -----------
----------1
1-----------------------
-----------------------1
1~~:=C-
Polluted
air intel
u,"WO"' _~)--:r
Figure 2.12. Schematic of a plate column.
3.2 ADSORPTION
In adsorption systems, the phases considered for mass transfer are a fluid and a solid.
As a matter of fact, when dealing with air pollution problems the fluid will be a gas.
Most solids are characterised by their capability to adsorb volatile compounds upon
their surface. However, the extent of adsorption does significantly vary from one
solid to another. Two adsorption mechanisms are possible, physical adsorption,
involving only weak forces of van der Waals and chemical adsorption or
chemisorption, involving a chemi cal reaction and formation of new chemi cal bonds
between the gas molecules and the surface of the adsorbent.
Physical adsorption is a reversible process because the forces between the
solid surface and the adsorbate are weak. The adsorbed volatile compound can thus
be desorbed and recovered, usually by thermic treatment. In the case of
chemisorption, true strong chemi cal bonds are formed and regeneration is more
difficult, leading most often to a modification of the chemi cal structure of the
adsorbent. Adsorption is an exothermic process, therefore adsorbed gas concentration
decreases as temperature is increased, when working at a constant pressure.
aluminas, silica gel, and molecular sieves. Table 2.1 summarises some typical
characteristics of these adsorbents. The data are only indicative and some variations
are possible, as a result of the wide variety of adsorbents belonging to the same
category. In some cases the adsorbent may be impregnated with a specific compound
which will react with the contaminant to be removed and enhance the removal
process, as in the case of NaOH impregnated activated carbon reacting with H2S
polluted air (Van Stone and Brooks, 1996). Adsorption is an efficient process only at
relatively low or moderate temperatures. At higher temperatures desorption will take
place or even destruction ofthe adsorbent (Table 2.1).
Activated carbon is obtained through thermic treatment of wood, nutshells,
carbon, peat, coal or other similar products. The porosity is significantly increased
after thermic treatment. Activated carbon, sold either in granular or in powder form,
is mainly used for the removal of organic compounds from contaminated air, the
process being suitable even in the presence of water. Most of the adsorption surface
is located in the pores (Figure 2.13). More information on activated carbon is also
given in Chapter 3.
Other adsorbents do usually preferentially adsorb water molecules. This is of
interest for drying air streams, though it becomes a major drawback when one wants
to remove organic contaminants from emis sion sources. In the latter case water must
be removed first. Activated aluminas are hydrated aluminium oxides obtained by
heat treatment. Silica gels are often used to remove sulphur. They are obtained by
neutralising sodium silicates with an acid solution. Salts are removed by washing
before drying and toasting the gel. Finally, molecular sieves or zeolites are
aluminosilicates possessing a crystalline and defined framework structure.
Adsorption does usually take place at the level of the cavity of each crystalline unit.
The pores leading to the cavity play a size-selective role for the molecules to be
Pore diameter
(10- 10 m) 10-100 20-130 20-40 3-20
Surface area
(m2/g) 500-1600 100-400 200-900 800-1000
Bulk density
(kg/m 3) 150-550 600-930 450-800 500-850
Thermal stability
(max. TO, 0c) 150 500 400 600
• • •• • • • •
adsorbed. More recently new or improved adsorbents have been used, among others
synthetic polymeric adsorbents (Anonymous, 1995) carbon fibers (Kenson, 1992),
catalytic/adsorptive carbon (Van Stone and Brooks, 1996), etc.
Activated Saturared
carbon bed activated
carbon bed
..-
Airout Water Vapor in
Decanter Decanter
(a) (b)
Figure 2.14. Schematic of an activated carbon contactor with steam recovery of the solvent.
x kC" (2.29)
q= M
where k and n are constants that can be obtained experimentally by measuring and
p!otting severa! values of q against C.
q=X/M
c
Figure 2.15. Typical adsorptioll isotherm.
36 C. Kennes el al.
x abC
(2.30)
q = M
(1+bC)
Many other equations may be useful in some specific cases for describing
some ofthe many possible isotherm shapes. The BET (Brunauer, Emmet and Teller)
equation is another example. Most isotherm equations are empirical or involve
numerous assumptions. Finding the equation that best agrees with the observed
isotherm is useful for modelling purposes and for predicting performance and
operation characteristics of adsorption beds.
Air inlet
Ca
Saturated_
~
zone
MTZ
C/Co
o
Volume of effluent treated (V)
Figure 2.16. Typical breakthrough curve and movement ofthe MTZ.
Non-Biological Technologies 37
2.16) and part ofthe pollutant will then progressively appear in the effiuent leaving
the column. The breakthrough point is reached when a specified percentage of the
influent concentration is detected in the column effiuent. A plot of the variation with
time of pollutant concentration in the effiuent leaving the bed is called a
breakthrough curve (Figure 2.16). Column exhaustion is reached shortly after
reaching the breakthrough point.
The time elapsed when reaching the breakthrough point or the service time
(ts) can be calculated from the breakthrough curve according to the following
equation:
(2.31)
(2.32)
Total height of the bed (HE) and bed height corresponding to breakthrough
(Hs) are related through the expression:
H
S
= (.!.s..)
tE
H
E
(2.33)
The height of the mass transfer zone is related to the shape of the adsorption
isotherm. It corresponds to the following equation:
HE - MTZ Hs (2.35)
t = =-
s v v
where v is the velocity of the MTZ flowing down the column. Such velocity is
usually quite lower than the linear gas velocity of air fed to the system.
3.3 INCINERATION
the concomitant rele ase of heat. If only partial combustion is reached, other
contaminants may be formed, such as organic acids, aldehydes, ketones, carbon
monoxide, etc.. In the case of halogenated pollutants an sulphur-compounds,
potential combustion products are S02, HCI and phosgene, among others
(Klinghoffer and Rossin, 1992; Freidel el al., 1993). It is worth underlining that some
combustion products might be more toxic than the original pollutant, as is the case
for phosgene generated during trichloroethylene incineration (Nimlos et al., 1993).
Reaching complete combustion is not always easy and depends on several
design factors, such as temperature, residence time (i.e., space velocity) and
turbulence (i.e., mixing) (Chu and Wu, 1998; Wang and Chou, 2000). A sufficiently
high temperature is required in order to allow fast ignition and combustion.
Combustion will start when the ignition temperature is reached. The addition of heat
is therefore needed. Once combustion has started, the oxidation process itself will
produce heat. If heat production is high enough combustion will go ono Such a
process is called direct flame incineration or direct combustion. Concentration of air
contaminants is often relatively low, meaning that heat production is also quite low.
If not enough heat is generated through oxidation, the addition of an external fuel
source is required and the process is called thermal incineration. In order to avoid
addition of fuel, a third alternative consists of using a catalyst which increases
reaction kinetics and allows lowering incineration temperature. Such a process is
called catalytic incineration. It allows reduc ing costs originating from the use of fuel.
However, catalysts are expensive and global costs will thus not necessarily be lower.
Although many VOCs are destroyed at temperatures around 600-700 aC,
thermal incinerators often need to be operated at temperatures close to 1000 aC, to
make sure combustion is as complete as possible and to avoid, whenever possible,
the formation of toxic or carcinogenic incineration products. Destruction of
halogenated compounds usually requires higher temperatures than the temperatures
used for non-halogenated aliphatic or aromatic molecules (Pope et al., 1976).
The level of completeness of oxidation also rei ies on residence time.
Residence time (t) is related to the volumetric flow rate ofthe feed gas (Q) and to the
volume ofthe oxidation chamber (V) through the following equation:
V (2.36)
Q
Figure 2.17. Thermal oxidation chamber used for treating 12000 m3/h of toluene
contaminated air (Courtesy ofKalfrisa).
Figure 2.18. Catalytic oxidation system for the treatment of industrial waste gases (Courtesy
of Kalfrisa).
Non-Biological Technologies 41
Polluted
air inlet
Fuel ~ ~ Air
andair ~ ~ outlet
Preheat
Catalyst
bumer
Polluted
air inlet
----. Air
outlet
takes place for different reasons, among which are thermal aging, clogging and
poisoning. Therefore catalysts need to be replaced periodically.
With thermal aging, the active surface area decreases with time as a result of
exposure of the catalyst to the reJatively high temperature of the gas. This may be
due to several factors, such as changes in surface structure owing to crystal growth
and narrowing or even closing of catalyst pores. Temperatures above 650 De are not
recommended (Siebert et al., 1984). Oxidation is an exothermic process and the
temperature reached in the incineration chamber should be checked carefully in order
to avoid destruction of the catalyst by heat produced dur ing operation. Clogging
occurs when the waste stream is contaminated with particles. Particulate matter
should therefore first be eliminated in order to avoid or slow down catalyst
deactivation. Poisoning results from the reaction of compounds, such as arsenic,
lead, zinc, phosphorus, sulphur, etc. at the level of active sites of the catalyst. Stable
products are then formed. impeding the reaction between air, volatile contaminants
42 C. Kennes et al.
3.4 CONDENSATION
Condensation is the conversion of a gas or a vapour into a liquid, when its partial
pressure is equal to the vapour pressure of the system. It is achieved either by
pressure increase or by lowering the temperature. For economical reasons the latter is
usually preferred. Combination of both temperature and pressure variations is also
possible. By pressurisation of air the molecules are brought closer together, while
lowering the temperature reduces the kinetic energy ofthe molecules.
Condensers are not very expensive and allow recovery and reuse of valuable
compounds. Cooling is often achieved with water or air, though other substances
could be used as well, depending on the characteristics of the waste gas and the
desired efficiency. However, temperatures below 30-40 aC are most oilen not
reached unless admitting increased costs. meaning that highly volatile pollutants will
most often hardly be removed. Therefore this technology is, in most cases, simply
used as a pre-treatment process useful mainly for VOC concentrations gre ater than
5000 ppmv and relatively low mass flow rates. Efficiency will drop at lower
contaminant concentrations or increased flow rates. In case VOCs get dissolved in
the coolant during condensation, pollutants will then be transferred from one phase to
another as was also the case in absorption and adsorption processes. The resulting
waste water then needs to be treated as well.
The heat exchange surface area is a key design factor. It can be obtained from
the heat exchange equation:
Non-Biological Technologies 43
Q=U A T m (2.37)
(2.38)
where
The overall heat transfer coefficient englobes the different individual heat
transfer coefficients and resistances. Conceming Tm, there are severa! means of
calculating the mean temperature difference in paralle! and counter-current shell and
tubes condensers. When the overall heat transfer coefficient remains constant and
when the heat capacity of each fluid is constant, the log mean temperature (Tim) may
be used:
(T2 -TI )
(2.39)
In(~)
where
44 C. Kennes et al.
TI = lowest temperature difference between the hot and the cold fluid
T2 = highest temperature difference between the hot and the cold fluid
If condensation is not linear and if the temperature range between hot and
cold fluid is large, lets say more than 20 aC, the log mean temperature should not be
used.
3.5.1. UVoxidation
In UV oxidation technology, a combination of oxygen containing oxidants, such as
ozone or peroxide, and UV light are used for the photochemical stimulation of
oxidation reactions, allowing the conversion of halogenated and non-halogenated
aliphatic or aromatic organic pollutants mainly into water and carbon dioxide. A key
design parameter is the UV light frequeney (200-280 nm) which is selected
aeeording to the nature of the VOC pollutants present in the waste air. Other faetors
playing a role in UV oxidation efticieney are waste air flow rate and temperature.
The reaction may take place in bateh or in continuous photoreactors. As aIready
mentioned earlier for ineinerators (Equation 2.36), flow rate is related to reaetor
residenee time through the following equation:
V=Qt (2.40)
where t is the reactor residence time, Q is the volumetric flow rate of the feed gas
and V is the active volume ofthe reactor.
Z
Treated air
Condenser
t
Air inlet
--.----+.\d~.
Compressor
~ I ~ I- - - - ' . 1 Membrane
unit
•
pump
Recycling
VOC
vacuum pump (Figure 2.22) creating a lower pressure on one side of the membrane
respective to the other enhances the separation process. Parameters goveming
treatment efficiency include waste gas flow rate and temperature, as well as VOC
concentration. Studies on the use of porous membranes in combination with gas
phase bioreactor technology have also been undertaken recently (Chapter 6) though
full-scale applications have not been reported so far.
References
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Air & Waste Manage. Assoc., 1995, San Antonio, Texas.
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Nimlos, M.R., Jacoby, W.A., Blake. O.M. and Miine. T.A. 1993. Direct mass spectrometric studies of
the destruction of hazardous wastes. 2. Gas-phase photocatalytic oxidation of trichloroethylene over
Ti0 2: products and mechanisms. Envrion. Sci. Technol. 27: 732-740.
Pope, O., Walker, O.S. and Moss, R.L. 1976. Evaluation of cobalt for the oxidation of low
concentrations of organic compounds in air. Atmos. Environ. 10: 951-959.
Prasad, R., Kennedy, L.A. and Ruckenstein. E. 1984. Catalytic combustion. CataI. Rev.-Sci. Eng. 26:
1-58.
Ruhl, M.J. 1993. Recover VOCs via adsorption on activated carbon. Chem. Eng. Prog. 89: 37--41.
Siebert, P.C., Meardon, K.R. and Serne, J.C. 1984. Emission controls in polymer production. Chem.
Eng. Prog. 80: 68-76.
Thomas, O. and Vanderschuren, J. 2000. Nitrogen oxides scrubbing with alkaline solutions. Chem.
Eng. Technol. 23: 449--455.
Van Stone, G. and Brooks, D. 1996. Carbon clean. Water Environ. Technol. February: 40--43.
Wang, J.B. and Chou, M.-S. 2000. Kinetics of catalytic oxidation of benzene, n-hexane, and emission
gas from a refinery oil/water separator over a chromium oxide catalyst. J. Air Waste Manage Assoc.
50: 227-233.
Wark, K and Warner, C.F. 1981. Air pollution, its origin and control. Harper & Row Publishers, New
York.
CHAPTER 3 CONVENTIONAL BIOFILTERS
1. Introduction
Most of the recent literature dealing with biological waste gas treatment indicates
that it is not really a new technology, which is indeed basically correct, taking into
account that biofiltration has been applied for several decades, though at small scale
and with low flow rates, mainly for the removal of volatile pollutants emitted from
waste water treatment plants and composting processes (Pomeroy. 1957; Ottengraf
and Diks, 1992). Biofiltration was initially mainly exc1usive1y used for the removal
of odours by means of soil biofilters designed and set up according to empirical
considerations. Applications have recently been extended to a much wider range of
compounds, mainly volatile organic compounds, over the last two decades.
Development of scientific studies, engineering concepts and non-empirical design of
biofilters is also quite recent, as well as the search for new support media and new
bioreactor configurations, as will also be described in following chapters.
2. Design of biofilters
47
C. Kennes and M. C. Veiga (eds.), Bioreactorsfor Waste Gas Treatment, 47-98.
© 2001 Kluwer Academic Publishers.
48 C. Kennes and M C. Veiga
Pretreatment
Air - .
inlet
---. Treated
Dram Water . - I (elean) air
water drainage ------'
The first biofilters which were built were open systems, meaning that the
upper part of the bioreactor was not c10sed (Figures 3.2 and 10.1). Although this
might present some relative advantage because of the natural supply of water in
moderately rainy regions, open bed biofilters are much more unstable than c10sed or
in-vessel systems. In closed biofilters (Figure 3.1), parameters, such as water supply,
water content, temperature, etc. are easier to control and regulate.
Pretreatment
Air - - .
inlet
Conditioned
air inlet
Drain
water
Empty bed residence time (h or s): it represents the mean residence time a
volatile compound would theoretically spend in an unpacked biofilter.
V
EBRT = t = - (3.1)
Q
In biofiltration the volumetric gas flow rate of bulk air (Q) may reach values
of up to 200000 m3/h (Kennes and Thalasso, 1998). It would not be surprising that
higher values might be reached as a result of improved reactor design and more
efficient operation. V is the packed volume (m3) of the reactor. If the re actor is not
packed, or, in other words, if it does not contain any carrier material, the active
reactor volume would correspond to the actual reactor volume available to the
substrate or to the bulk air flow. However, in packed reactors such as conventional or
trickling biofilters, air can only occupy the void volume which depends on, among
others, the porosity ofthe carrier.
50 C Kennes and MC Veiga
(3.2)
where e is the ratio between the void volume available to air and the total reactor or
carrier volume.
Since it is not easy to accurately estimate the value of e, the EBRT is the
parameter most often used in biofiltration and most frequently reported in the
literature. Values of e are not necessarily identical to porosity values, for instance
when the air flow is unable to reach some pores.
Typical EBRT values are close to 1 minute, although some biofilters may
successfully be operated at residence times ranging from less than half a minute to
several minutes (Table 3.1). However, full-scale conventional biofilter operation is
often not cost effective for EBRT exceeding one minute. The influence of the EBRT
on biofilter performance is also illustrated in Figure 3.3.
-
o~
>.
(,)
t:
100 • • •
Q) 80
'0 •
!EQ)
ca 60 •
>
O
E
Q)
40
e:::
20
O 2 4 6 8 10 12 14 16 18
Gas residence time (min)
Figure 3.3. Influence ofthe EBRT on biofilter performance (Hwand and Tang, 1997),
(reproduced with permission).
R= (3.3)
Conventional Biofilters 51
where Vs and vp are the average bulk air velocity (mlh) and the mean pollutant
velocity (mlh), respectively.
The retardation factor may be calculated by using a pulse experiment
consisting of introducing a spike of contaminant at the inlet of the biofilter and
measuring the movement of the pulse passing through the filter bed (Hodge and
Devinny, 1994). The retardation effect may be attributed to a series of factors often
grouped under the term adsorplion because adsorption is one of the main processes
involved in this phenomenon. Pollutants may indeed be adsorbed onto the carrier
material and to the biofilm, including the microorganisms and ali other material
related to the biofilm, as exopolymers produced by the biomass. However,
contaminants are also absorbed and retained in the aqueous phase, otherwise their
biodegradation would not occur, since microorganisms are active in the aqueous
biofilm or in suspension in the free water film. Under ideal conditions, at equilibrium
the amount of pollutant in the water phase is related to the contaminant concentration
in the bulk air through Henry' s law' s constant. Thus numerica! values of the
retardation factor basically depend on the time pollutants will remain adsorbed onto
solids and/or absorbed in the aqueous phase. To give an idea of orders of magnitude,
retardation factors reported for a compost biofilter and an activated carbon biofilter
reached, respectively, values of 3600 and 26000 (Hodge and Devinny, 1994).
Table 3.1. Typical EBRT used for treating different poliutants in conventional biofilters
.
gsl m3 .h, E.C. = Elimination Capacity
Veiga el al., 1999
Superficial gas velocity (m/h) Of surface loading rate: It re~resents the ratio
ofthe gas flow rate (Q, m3/h) to the surface area ofthe carrier (A, m ).
Q (3.4)
v,
A
52 C. Kennes and M C. Veiga
Volumetric loading rate: The volumetric loading rate is the ratio of the gas
flow rate (Q, m 3fh) to the total volume ofthe filter bed (V, m\
Q (3.5)
v =-
I V
Surface (m 3/m 2 .h) and volumetric (m 3/m 3 .h) loading rates are typically in the
range of about 60-180. However, quite lower or higher values have successfully
been used as well. Volumetric loads of 7 or 8 m 3/m 3 .h have been reported both for
the removal of odour from waste water treatment plants and for VOC biodegradation
in full-scale plants (van Groenestijn and Hesselink, 1993). Higher values reaching
426 m 3/m3 .h were applied in the pilot-scale removal of formaldehyde in plywood
production plants (van Groenestijn and Hesselink, 1993). Surface loads as high as
500 m 3/m2 .h have been applied in a compost-bark biofilter while managing
maintaining low pressure drops (Leson and Winer, 1991).
Substrate mass loading rate (g/m 3 .h): The substrate mass loading rate is the
mass of contaminant fed to the biofilter per unit time and unit volume of carrier
material,
V
Q Sin
=-- (3.6)
v V
Elimination capacity (g/m 3 .h): The eJimination capacity (EC) is the amount of
substrate ar pollutant the biofilter is able to remove per unit volume of carrier
material and unit time. Its mathematical expression is given below.
EC
Q (Sm - SOli') (3.7)
V
Elimination capacity and mass loading rate are both usually expres sed in
g/m 3 .h or mg/m 3 .h. However, pollutant concentrations are sometimes given in g/m 3
or in ppmy. Both units are related and conversion is straightfarward (Chapter 1). If
the substrate concentration is given in ppmy and if the elimination capacity under
standard conditions needs to be expressed in mg/m 3 .h, the following equation will be
used:
EC = 24 5 Q (Sin - SpUI) (3.8)
. MWV
Conventional Biojilters 53
(3.10)
~80-.------------------------------.
-
..,'
E 70 -
~ 60-
:5 50
iti
g. 40
u
s:: 30
O
:;; 20 -
s::
:§ 10-
W O -~------~---------,---------,--~
O 40 80 120
Mass loading rate (g/m 3 .h)
Figure 3.4. Typical plot ofTEX (toluene, ethylbenzene, o-xylene) elimination capacity
versus mass loading rate in a perlite-biofilter (non published data).
54 C. Kennes and M C. Veiga
(3.12)
RE
QS lI1
When plotting mass loading rate versus EC with identical scales and units on
both axes a straight line with a slope = 1 will rcpresent a 100% removal efficiency
(Figure 3.4).
2.3.2. Modelling
Reactor model equations are useful tools for calculating expected biofilter
performance as well as for scaling-up purposes. Basic concepts used in reactor
modelling are based on fundamental engineering equations valid irrespective of the
type of reactor. These equations are (bio )reaction rate equations and continuity,
energy and momentum equations (Froment and Bischoff, 1990). In the first model
applied to the treatment of polluted air in biofilters, equations used for modelling
biofilm-reactors mainly designed for waste water treatment (Harremoes, 1978;
Rittman and MacCarty, 1980) were initially adapted to biofilters for air pollution
control (Ottengraf, 1986). Such model equations have been used for many years.
They are based on simplifying assumptions presenting some limitations, although
they have successfully been applied on several occasions to lab-scale reactors and for
designing full-scale biofilters operating in different countries. Efforts have bccn
made very recently, since the early nineties, to improve biofiltcr models and several
research groups have proposed new alternatives. Although different models
described in the literature will briefly be explained, the simplest and first proposed
model (Ottengraf, 1986) will be detailed more cxtensively since it is at present sti II
the most popular choice. It is also worth noting that several of the more sophisticated
and more recently proposed model equations are, to some extent, based on that first
model or on similar equations.
2.3.2.1. Bioreaction rate equations. Although both resting cells and growing
microorganisms may be involved in the biodegradation of volatile compounds in
continuous gas phase biofilters, in aqueous batch assays mineralization of volatile
organic compounds is typically a growth Iinked biodegradation process. Under such
conditions, microbi al growth rates and removal rates of pollutants are Iinked through
the biomass yield or mass of cells produced per mass of pollutant degraded (Y XlS)
(g/g). An example of growth related biodegradation is shown in Figure 3.5 for a
Pseudomonas strain used as inoculum in biofiltration studies (Amor et al., 2001).
Some typical values ofbiomass yields for microorganisms found in gas-phase
biofilters are presented in Table 3.2. Parameters used in microbial kinetic equations
(see below) may therefore be evaluated in batch assays either by following
biodegradation patterns or growth rates.
Conventional Biofilters 55
50 0.6
...
-
.............. __
0.5
40
1 ,
--
--
I
I
...J
0.4 I
30 E
-
Cl
E 0.3
1::
o
U)
al
1::
al
20 ~
:::l 0.2 ci
"O O
1-
10 0.1
O O
O 20 40 60 80 100 120
Time (h)
Figure 3.5. Example of growth related biodegradation of toluene by a Pseudomonas sp.
(Amor et al., 2001).
Table 3.2. Typical biomass yields (Y XIS) and Ks and K, values for Pseudomonas spp. grown
on alkylbenzenes in liquid phase batch culture
Pseudomonas sp. 18.9 161.2 0.55 TEX (1:1:1) Veiga el al., 1999
Pseudomonas BI 1.96 1.22 Toluene Chang el al., 1993
Pseudomonas XI 0.99 1.88 Toluene Chang el al., 1993
P. putida 0.1 1.2 Toluene Pedersen el al.,
1997
P.putida 6 1980 0.6 Toluene Choi et al., 1992
TEX = Toluene + Ethylbenzene + o-Xylene
Supposing that the growth rate depends only on the concentration of one
compound (S), the Monod equation then takes the following form:
56 C. Kennes and MC. Veiga
S \
f1 = f1 max
(
Ks + S) (3.13)
Ks is the substrate concentration that gives half the maximum growth rate. It
represents the affinity of a given microorganism for the substrate S. The value of Ks
must be known if one wants to use Monod' s equation for solving biofilter modelling
equations. Accurate estimation of Ks values is often not easy since biofilters are
usually colonised by mixed, often unidentified microorganisms, rather than by one
single strain. AIso, depending on the method used, quite different Ks values may be
obtained for a same microbi al strain using Monod's model (Table 3.3). Kinetic
parameters may vary in some cases by up to one order of magnitude for a given
strain, which is non negligible in designing problems and biotilter sizing.
Table 3.3. Example of variable Ks values obtained with Xanthobacter autotrophicus GJI0
grown on 1,2-dichloroethane (Ferreira Jorge and Livingston, 1999)
(3.15)
In such case, microbial growth rate (Il) and biodegradation rate (rs) in
biotilters are proportional and are related through a constant value according to:
if one assumes that biomass yield (YX/s) and biofilm density (B) are constant
parameters.
Conventional Biojilters 57
2.3.2.2. Simple steady state biojilm reactor model adapted to conventional biojilters
for air pollution control. The model is based on mass balance equations. As
mentioned below, several assumptions need to be made for this simple biofilter
model:
Substrate mass balance equations need to be written both for the biofilm and
for the bulk gas phase. Under steady state conditions the biofilm mass balance
equation is:
o Dd2SJ
(dx 2
- Reaction rate (3.17)
with
D = effective substrate diffusion coefficient in the biofilm (m 2!h)
= effective substrate diffusion coefficient in water (m2!h)
x = biofilm depth (m)
The reaction rate is calculated from the Monod equation as explained above.
In order to obtain an analytic solution, the Monod equation needs to be simplified
and reduced either to a zero order or a first order expres sion as described previously.
Sg (3.20)
H
(2) dS b = O (3.21)
dx
where
Sb = substrate concentration in the biofilm (g/m3 )
Sg = substrate concentration in the bulk gas phase (g/m 3 )
H = Henry's law's coefficient (-)
The mass balance equation for the bulk gas phase along the biofilter height
under steady state conditions is:
where
u = superficial gas velocity (mlh)
= Q/A = gas flow rate (m3/h) / empty bed cross sectional area (m 2)
h = reactor height (i.e., carrier height) (m)
As = biolayer surface area per unit volume of bioreactor (m 2/m 3)
N = flux of substrate from the gas phase into the biofilm (g/m 2 .h)
= _D (dS b )
dx FO
Thus
(3.23)
(3.24)
meaning that the substrate concentration (Sg.h) at height h = O is equal to the substrate
concentration in the feed (Sg.o).
The set of equations may easily be solved for three different operating
regimes as mentioned hereafter, obtaining new equations relating the feed
concentration to the pollutant concentration at different heights in the biofilter
(Ottengraf and van den Oever, 1983).
Conventional Biofilters 59
A.l) Zero order reaction (biodegradation) rate with substrate difJusion limitation
(Figure 3.6).
(3.25)
2dS)O.5
o= (--g (3.26)
ko H
A.2) Zero order reaction (biodegradation) rate with reaction limitation (Figure 3.6).
(3.27)
where o' is the effective biotilm thickness. The biotilm is m this case fully
penetrated.
z
Figure 3.6. Pollutant concentration for zero order kinetics with either diffusion limitation
(Al) or reaction limitation (A2) and for tirst order reactions (8).
B) First order reaction (biodegradation) rate. For a tirst order reaction, the Thiele
modulus is used to distinguish between diffusion limitation and reaction limitation.
60 C Kennes and MC Veiga
~=o' --t
( k ) 05 (3.28)
The gas phase substrate concentration profile along the height of the biofilter
is calculated from:
C) Improved models. One of the major advantages of the above mentioned model is
that it yields simple equations for which analytical solutions are quite easily
obtained, Although it is based on a series of simplifying assumptions, it often leads
to a good fit between model equations and experimental data, However, in some
cases, such as when working with mixed waste gases or in the case of uneven
biomass distribution, the model equations may not fit experimental data (Veiga and
Kennes, 2001a), Therefore efforts have been made very recently for developing
improved model equations (Devinny et al., 1999). Such models are considered to be
improved models in that they are usually a closer picture of the real situation.
However, in most cases they are more complicated to use and to apply and no
analytical solution is available,
CI) Bioreaction rate equation. Pollutant concentrations are prone to vary over time
in industrial waste gases. Contaminant concentrations do also vary with biofilter
height since the pollutant gets gradually biodegraded as the air stream passes through
the reactor. According to Monod kinetics biodegradation rates may thus switch from
zero order to first order kinetics, Such transition is not instantaneous and fractional
order kinetics may be observed over part of the total biofilter height. It is therefore
more logical to use the Monod equation (Hirai et al" 1990; Deshusses et al., 1995a)
or to switch from zero order to first order kinetic equations at a given reactor height.
Also, at high pollutant concentrations, it will be more accurate to use kinetic
equations which take into account possible inhibitory effects, such as the Haldane
equation or the Andrews equation (Andrews, 1968; Shareefdeen el al" 1993;
Shareefdeen and Baltzis, 1994). The Andrews equation has the following form:
S
(3.30)
When several pollutants are present in a waste gas, model equations considering
cross-inhibition effects may be necessary (Baltzis and Shareefdeen, 1993; Deshusses
et al., 1995a, 1995b).
C2) Limiting substrate. Substrate concentration (S) in the kinetic equation refers to
pollutant concentration. However, in some cases oxygen might become limiting in
biofilms and control the overall removal rate. In such a case the oxygen
concentration needs to be inc1uded in the kinetic expression (Shareefdeen et al.,
1993). Possible kinetic equations are then:
(3.31 )
li = limax (K SP
or
(3.32)
C3) Non-steady state conditions. Biofilters are most likely to be operating under
non-steady state conditions, among others as a result ofthe variable characteristics of
industrial waste gases over time. Model equations taking into account such transient
states have been proposed and described by few authors (Shareefdeen and Baltzis,
1994; Hodge and Devinny, 1995; Deshusses et al., 1995a, 1995b; Devinny et al.,
1999).
C.4) Other parameters. Comments on other assumptions need to be made. The use of
water/air partition coefficients for calculating pollutant concentrations in the gas
phase and in the biofilm may not be valid in some cases, mainly when working with
hydrophobic pollutants (Mohseni and Allen, 2000).
Another key factor to be considered when modelling is that homogenous
quantitative and qualitative biomass distribution is generally assumed. It is quite
obvious that in natural carriers (soil, peat, etc.) this might not be true. Recent studies
have also shown that with other carriers (perlite, celite) biomass concentrations do
vary along the biofilter. Higher microbial concentrations are found near the inlet of
the reactor (Cox et al., 1997; Song and Kinney, 2000a, 2000b; Veiga and Kennes,
2001a). Up to 20% (Cox et al., 1997) or even 40% (Veiga and Kennes, 2001a) more
biomass may develop near the entrance of the system. Aiso biofilm or biomass
activity is sometimes not homogenous along the reactor height (Veiga and Kennes,
2001a) and is expected to vary with time, for instance, in the presence of variable
microbial populations. In case such variations would not be negligible, mass balance
equations should be applied to the biomass. As will be commented further in this
chapter, it was recently also shown that shifts in microbial populations are expected
to occur in conventional biofilters, even for relatively short periods of operation of a
few months (Sakano and Kerkhof, 1998; von Keitz et al., 1999).
62 C. Kennes and M C. Veiga
Gas flow rate and feed composition are of prime importance in biofiltration. Besides
mass transfer rates, global removal rates or e1imination capacities are highly
dependant on biodegradation rates. Both mass transfer rate and biodegradation rate
are affected by the composition and other characteristics of the feed. At higher gas
flow rates, resulting in shorter residence times deeper biofilters will be needed. Feed
composition will affect reactor sizing as well. Usually larger biofilters will be
required when dealing with higher substrate concentrations or in the case of highly
reca1citrant compounds. One of the main advantages of biofiltration compared to
other technologies is its low cost. However, when larger biofilters are used,
investment costs do increase.
As a general rule biofiltration technology is often not the best choice for
pollutant concentrations above 4 or 5 g/m3 ; on one hand, because it would increase
investment costs and, on the other hand, because of potentially inhibitory effects on
biomass activity. Inhibitory effects observed at high pollutant concentrations or
during shock loads may partly be buffered and avoided by using carrier materials
with high adsorptive capacity, i.e., activated carbon (Devinny and Hodge, 1995;
Weber and Hartmans, 1995). Unless working at high EBRT, biofiltration at relatively
high substrate concentrations may lead to low removal efficiencies (Table 3.4) and
accumulation of toxic intermediate biodegradation products (Devinny and Hodge,
1995). Although relative1y high elimination capacities may be reached, residual
concentrations released from the bioreactor effluent might not comply with
regulatory requirements. Higher mass loading rates would also generate higher
temperature increases resulting from increased metabolic activity. When dealing with
highly loaded waste gases, biofiltration could stiU advantageously be used by
combining this technology with other non-biological processes.
Table 3.4. Influence ofthe feed concentration on the removal efficiency of some VOC s
Biofilter performance is highly dependent on the nature of the carrier material, also
called filter bed, support material or medium by different authors. The carrier
material is a solid phase on which adhesion of the biocatalyst (microorganisms) takes
place resulting in the development of a so called biojilm growing as a result of
pollutant degradation.
Compost. Although soil was probably the first natural filter medium used in
biofiltration, compost and peat gradually gained better acceptance later on and they
are nowadays probably the most popular non-synthetic carriers. Composting is a
technology used for the aerobic or, sometimes, anaerobic biologic al conversion and
stabilisation of organic matter mostly present in solid form. As a result of the
biological activity and the solid nature of the system, thermophilic conditions are
reached leading to a product free of pathogens. Aerobic composting is usually
preferred over the anaerobic process since end products of anaerobic conversion
generate odour problems which are, contrarily, basically avoided under aerobic
conditions.
64 C Kennes and M C. Veiga
filter bed is that it might not be free of organic contaminants or heavy metals (Martin
and Loehr, 1996) causing inhibition of microbial activity. Many prime matters are
suitable for composting. Some examples are bark, different kinds of sludges, yard
trash, wood residues and agricultural wastes. Composts produced from such
substrates have already ali been used in biofiltration studies (Morgenroth et al., 1996;
Smet et al., 1996; Tang et al., 1996). A wide variety of microorganisms is found in
compost inc1uding bacteria, fungi (yeasts and molds), algae, protozoa and virus
partic1es. A wide microbial flora will thus naturally be present on start-up of
biofilters using such a filter bed, although they might sometimes not possess the
enzymes needed for mineralization of recalcitrant contaminants present in polluted
air streams.
and Manu-Tawiah, 1989): total solids, 19.50 ± 0.50, total lipids, 2.52 ± 0.17, total
nitrogen, 0.80 ± 0.08. The moisture content of wet peat was around 80.50 % with a
pH of 4.85 ± 0.11. It also contains carbohydrates and trace minerals. A typical
elemental analysis ofpeat is (%) (Hirai etal., 1990): C, 48.03; H, 5.51; N, 0.82; S.
0.21; Fe, 0.12; ash, 4.20. In this case water content was 46.7% and pH 3.75. Peat is
in most cases acidic.
Soi/o Most of the first biofilters used for air pollution control were open soil
biofilters. Polluted air was simply passed through soil either in an underground or
above ground biofilter taking advantage of the natural presence of soil
microorganisms able to degrade the contaminants. Viable heterotrophic plate counts
per gram dry weight of fertile soil have been reported as 10 8_10 10 bacteria and 10 5_
108 actinomycetes (Alexander, 1977). Dry soil is composed both of inorganic
mineral compounds and organic matter. Wide variations may be found in the ratio
between these two components and the organic maUer content may vary from less
than 1% to about 95%. Some characteristics of soils used in biofiltration are
presented in Table 3.7 (Miller and Canter, 1997). Moist bulk density does usually
range between the density of soil organic maUer (about 0.5 g/cm3) and the density of
mineral matter (about 2.7 g/cm\ Contrary to several other natural carriers, inorganic
soil is hydrophilic. It is usually less sensitive to fluctuations in moisture content but
its low permeability often leads to significant pressure drops over long term
operation periods and to the need ofusing large EBRT.
3.3 MICROFLORA
months (Cox et al., 1997; Veiga and Kennes, 2001a). This is particularly true when
defined inocula are used with synthetic carriers and if native microorganisms present
in such inocula were directly enriched in bioreactors fed with specific VOCs. In
other cases inoculated strains might get overgrown by other more performant
organisms (Fritsche and Lechner, 1992; Jorio et al., 1998). Biofilter inoculation may
also represent a means to speed up the start-up period (Veiga and Kennes, 2001a),
even though inoculated microorganisms might eventually get overgrown by other
strains in the long run. Examples of pure cUltures or defined mixed cultures used for
inoculation of conventional biofilters are presented in Table 3.8.
For biofilter inoculation with pure cultures, speciali sed bacterial inocula are
normally used. Recent research studies have shown that seeding eukaryotes as fungi
or algae might be useful in some cases. Studies on the biodegradation of VOCs by
fungi were reported already several decades ago (Anselmo et al., 1985; Edmonds and
Cooney, 1967; Engelhardt et al., 1977; Goldbeck el al., 1983). The removal of
sulphur compounds, such as hydrogen sulphide, methanethiol and dimethyl sulphides
by fungi has also been reported, yielding sometimes higher biodegradation rates than
with bacteria (Phae and Shoda, 1991). Studies on the use of fungal inocula in wastc
gas treatment were started more than ten years ago and were first published in the
late eighties and early nineties (Hiittermann et al., 1988; Majcherczyk et al., 1990;
Braun-Liilleman et al., 1992; Cox et al., 1994). White rot fungi are very popular
organisms in biodegradation studies. Although they have proven to be best suited for
the co-metabolic removal of semi-volatile complex aromatic substrates, such as
polycyclic aromatic hydrocarbons (Cemiglia, 1992) rather than highly volatile
substrates, some researchers suggested their use in biofiltration ofVOCs.
A potential problem with white rot fungi is the accumulation of intermediate
products (Kennes and Lema, 1994; Yadav and Reddy, 1993), although relatively low
molecular weight metabolites might get degraded by other microorganisms in
complex cultures as found in biofilters. Biofiltration studies undertaken in the
presence of strains, such as Trametes versicolur, Phanerochaete chrysusporium,
Pleurotus ostreatus and Bjerkandera adus ta using lignocellulosic materials (straw,
agricultural residues, etc.) as filter bed, allowed reaching high elimination capacities
for compounds, such as a-pinenc, styrenc and alcohols, with sometimes complete
conversion to carbon dioxide and water, which should most probably result from the
metabolic activity of other microorganisms present in filter bed next to these
basidiomycetes (Braun-Liillemann et al., 1992). Since most white rot fungi de grade
lignocellulosic material, i.e., the filter bed, studies on bed compaction and
concomitant pressure drop would be useful.
As a general rule fungi may be especially suitable for the removal of
hydrophobic pollutants, such as styrene or alkylbenzenes (van Groenestijn and
Hesselink, 1993). In biofilters the aerial hyphae of fungi represent a large surface
area in direct contact with the contaminated gas phase (Braun-Liillemann et al.,
1992). Under such conditions absorption of hydrophobic compounds is favoured
since the contaminant is directly transferred to the cell surface without phase
transition problems. Other interesting characteristics of most yeasts and filamentous
fungi are their resistance to extreme environmental conditions, such as low water
contents and low pH values although their metabolic activity under such conditions
may be reduced. Although the first reported studies were undertaken with natural
carriers and white rot fungi (Majcherczyk et al., 1990; Braun-Liilleman el al., 1992),
probably because they are well characterised and widely used strains, other fungi
~
Table 3.8. Examples of pure cultures or defined mixed cultures used in conventional biofilters
grown on inert carriers might be more performant (Cox et al., 1994, 1997).
Good reactor performance was obtained with a biofilter containing the fungus
Exophiala jeanselmei forming long filamentous mycelia. The latter strain uses the
pollutant as the sole source of carbon and energy and biodegradation does not rely on
the rresence of a co-substrate. Maximal styrene elimination capacities around 62-90
g/m .h were reached (Cox et al. , 1997). Similar results were obtained in the presence
of an alkylbenzene degrading culture composed of mixed populations of bacteria,
yeasts and filamentous fungi (Figure 3.7) (Veiga et al., 1998; Veiga and Kennes,
2001a). Some examples of yeasts and fungi inoculated in vapour phase bioreactors
appear in Table 3.9. Fungal strains inoculated in biofilters for VOC treatment should
preferably possess the following characteristics (Sanchez-Pefia el al., 2000) :
Figurc 3.7. SEM photograph of carrier material from a biofilter treating alkylbenzenes
showing the presence of numerous fungi and bacteria (Veiga and Kennes. 200 I b).
Table 3.9. Some characteristics and performance of biofilters inoculated with fungi
3.3.3.1.Techniques for cel! counts. Different methods have been used for
enumeration of cells and for evaluating attached biomass concentrations in
conventional biofilters. In most cases, the first step consists of suspending a given
amount of carrier in a known volume of aqueous phase. The composition of such
aqueous phase may vary depending on the purpose and the research group. The
sample is then treated. Here again, different alternatives have been used, such as
grounding and later vortexing the sample for supernatant analysis (Wu et al., 1999)
or sonication of the sample (Cârdenas-GonzaJez et al., 1999; Veiga and Kennes,
2001a). After serially diluting the suspension, aliquots are spread on plates allowing
counting specific microbial groups on selective media. Specific inhibitors and
antibiotics may also be used if necessary (Veiga el al., 1997). If one wants to
evaluate the total amount ofbiomass attached on the support, this may be checked by
different techniques, such as estimation of dry mass content or protein concentration.
3.3.3.2. Cel! counts in biojilters. Data have been reported on cell counts in biofilters
containing either organic or inorganic carriers. Cell counts obtained in biofiltration
studies using several composts as natural carriers are reported in Table 3.10
(Cârdenas-Gonzalez et al., 1999). The biofilters were used for the removal of a
74 C. Kennes and M C. Veiga
or CSHs3N01.3S for bacteria or C4 H7N o.6 02 for yeasts although vanatlOns are
observed, depending on the species. Therefore such elements need to be available to
the microorganisms. Other important nutrients and trace elements include mainly S,
P, K, Mg, Ca, Fe, Mn and vitamins which may be required by some species.
Phosphorus and potassium may represent up to 5 % of the dry cell weight.
Nutrients are naturally present in organic filter beds although not necessarily
in balanced ratios. This is not the case with most inert and synthetic carriers where
addition of nutrients is always required. It is also worth mentioning that nutrients get
gradually depleted in biofilters packed with natural carriers. After a given period of
operation, addition of nitrogen has shown to improve biofilter performance in the
case of carriers, such as wood bark (Weckhuisen et al., 1993), peat (Arnold el al.,
1997), compost (Morgenroth el al., 1996) or compost-perlite media (Gribbins and
Loehr, 1998). In the latter case, elimination capacity increased from 25 to gre ater
than 100 g toluene/m 3 .h. If increasing nutrient concentration will, to some extent,
improve elimination capacities (Wu el al., 1999), it will nevertheless also enhance
microbial growth and favour pressure drop increase. Although the addition of
nutrients will increase operation costs, it should be taken into account that if such an
addition improves the removal efficiency, smaller biofilters can be used, resulting in
reduced investment costs. It is also expected that natural carriers might be used for
longer periods of time before requiring replacement as a re suit of nutrient depletion.
If the availability of nitrogen, phosphorus, etc. in the biofilter is important,
the form in which it is present is important as well. For instance, the presence or use
ofNH4 CI in non-buffered media willlead to pH drop, since microorganisms will use
nitrogen for growth, resulting in the release of a proton in the medium. A typical
example of methanol biodegradation in presence of ammonium chloride, considering
CSH9N02S as the biomass composition, is given below showing the re1ease of HCI
resulting in medium acidification (Shareefdeen el al., 1993):
Biomass yield, or the amount of cell mass produced per mass of nutrient or
substrate consumed, is also dependent on the nature of the nutrients. Here again,
ammonium will yield higher amounts of cells than, for instance, nitrate (Moo-Young,
1985). When considering toluene as substrate, theoretical biomass yields calculated
based on energetics relationships have been reported to reach 1.26 g biomass / g
toluene and 0.77 g biomass / g toluene, respectively, with ammonia or nitrate as
nitrogen source (Gribbins and Loehr, 1998). However, experimental results may lead
to quite lower yields (Choi el al., 1992; Veiga el al., 1999).
Oxygen is another important substrate naturally present in air. It is required
for the aerobic biodegradation of pollutants. Oxygen concentration needed for
pollutant removal is, in many cases, available in excess (Deshusses el al., 1996),
although it seems that it could become limiting when working at high substrate 10ads
and/or in presence of thick biofilms. Biofilters treating styrene at influent substrate
concentrations around 2.2 g/m3 and a volumetric load of 90 m3/m 3 .h proved to
perform better when working with air enriched with 40% oxygen than in presence of
only 20% O2. For otherwise identical operating conditions, e1imination capacities
were, respectively, 91 and 62 g/m3 .h (Cox el al., 1997). Other authors (Baltzis and
Shareefdeen, 1994) also showed that oxygen might get depleted faster in the biofilm
than the target pollutant, but here again this should also depend on, among others,
76 C. Kennes and MC. Veiga
3.5 WATERCONTENT
mass ofwater
Water content (wet)
mass of water + mass dry carrier
mass of water
Water content (dry)
mass of dry carrier
and high water activities, temporarily feeding dry air to the reactor would probably
damage the external layer of the biofilm and temporarily reduce overall biofilter
performance. The effect of the water content or water activity depends on the nature
of the carrier material. More water is adsorbed and bound to the filter bed in the case
of natural organic supports than with inert carriers, suggesting that less water is
available to microbes in the former than in the IaUer (Bohn and Bohn, 1999).
Most nutrients required by the micro flora found in biofilters are available in
the liquid layer present either in the biofilm itself or otherwise next or close to it. One
of the major differences between conventional biofilters and biotrickling filters is the
presence of a thicker water layer in the IaUer system meaning also an extra mass
transfer resistance (Kennes and Thalasso, 1998). In fact, a free water film may also
be present between the gas phase and the biofilm in conventional biofilters.
Neverthe1ess such film is very thin and basically negligible. Thickness of the water
film on surfaces of inorganic carriers has been estimated to be less than 10 nm (Bohn
and Bohn, 1999). This is about 50 to 5000 times less than the diameter of bacteria or
fungi. In conventional biofilters contrary to biotrickling filters the water layer is
stationary. In both reactors, flow of bulk air is turbulent and, in that region, mass
transfer of pollutants takes place by convection. Contrarily, air flow near the air-
water interface is laminar and, there, the pollutant is transferred by molecular
diffusion which is a slower mass transfer process than convection. Nevertheless,
molecular diffusion is usually not a rate limiting step as the water film is almost
negligible in conventional biofilters.
-
..c: 100
1
--
C')
r •••
E 75 0.75 ~
CD .:;
o::: 50 0.5 ~
--
fi) 10
.s10
~
o~ 25 0.25 ~
O
== O O
O 0.25 0.5 0.75 1
Distance in filter bed (m)
Figure 3.8. Water content (WC, e), water activity (.) and elimination capacity (SR,--)
versus reactor height in a biofilter treating styrene vapours (Cox el al., 1996), (reproduced
with permission).
reaching the inlet port of the biofilter. Saturation levels near 95% are usually
reached, though this will usually not be enough to compensate for water losses
resulting from, among others, volatilisation, enhanced by temperature increases
resulting from microbial activity. Ideally, relative humidity of influent air should
exceed 99% and be as close as possible to 100% since in a such case, theoretically,
air passing through the biofilter could not adsorb any additional water from the filter
bed unless temperature is increased. An aqueous solution often needs to be sprinkled
on top of the reactor as additional moisture regulation since 100% humidity is often
not reached by mere pre-humidification. If required such liquid solution will contain
nutrients, above all in case ofworking with non-natural carriers.
A water content of 40-60% seems to be adequate in many applications and
for most carriers, as shown in Figure 3.9 for a conventional biofilter packed with
perlite (Veiga and Kennes, 2001a). In the latter reactor, the water content remained
in the range 40--60% for at least one month simply by feeding an air stream passing
through a humidification chamber, without the external addition of any aqueous
phase through a separate circuit (Veiga and Kennes, 200Ia). Such water retention
capacity of inorganic carriers also explains why inert hydrophilic carriers, such as
perlite or ceramic can be used in conventional biofilters and not only in trickling
bioreactors. However, depending on the nature of the carrier material, slightly higher
or lower water contents seem to be suitable (Kennes and Thalasso, 1998). Some
examples are the treatment of sulphur compounds in peat biofilters operated at a
moisture content around 70--74% (Hirai el al., 1990) or the removal of propane by
soil beds at a water content of only 20% (Ebinger et al., 1987). The suitability of
such high or low water contents does not necessarily mean that these values are
optimal. Optimal water content is governed to agreat extent by the physical
characteristics of the carrier material, such as the pore size. Water in very small
micropores is hardly available to microorganisms.
--
~
o
>- 80
100
(J
r::::
CI)
'0
it:CI) 60
ca
>
O 40
E
CI)
o::
20
20 30 40 50 60 70
Water content (%)
Figure 3.9. Influence of water content on removal efficiency 111 a biofilter treating
alkylbenzene vapours (Veiga and Kennes, 2001a).
Conventional Biofilters 79
Too high a water content will lead to the formation of stagnant zones with
mass transfer limitation, possible anaerobic conditions owing to poor oxygen
transfer, and increased pressure drop. Increasing moisture content also results in
heavier drain water leaching. Too Iowa water content or water activity will reduce
microbial activity although some microorganisms, such as fungi are more tolerant
than others to such conditions. Although most often water activities above 0.9 seem
to be required for bacterial activity, fungi tolerate lower values. Many yeasts and
filamentous fungi are metabolically active at water activities around 0.80 or less. In
the case of hydrophobic compounds, such as a-pinene it was observed that a low
water content increased pollutant concentration in the wet biolayer up to toxic levels
(Apel et al., 1995).
The initial moisture content of the carrier material on starting-up the system
seems to be another relevant factor. Media which are not sufficient1y moistened
when preparing the packing might not retain enough water later on and might never
reach a high enough moisture content to ensure optimal operation. Compost-perlite
biofilters started-up at water contents of 0% and 20% and continuously fed a
humidified gas stream (95% humidity) reached, respectively, water contents of only .
4% and 9% at equilibrium which is far too low (Quinlan et al., 1999). As a general
rule, natural organic carriers are more sensitive to water content variations than inert
or inorganic carriers, among others because the structure of most natural carriers will
(sometimes irreversibly) change during drying periods impeding proper rewetting
later ono A similar problem was reported in case of a peat biofilter treating ethanol
vapours (Auri a et al., 1998). Carrier materials with hydrophobic surfaces like
compost have high air-water-solid contact angles making them difficult to rewet
when dry (Bohn and Bohn, 1999; Kraislas et al., 2000). This is also true for peat,
wood chips, activated carbon, etc. Such hydrophobic surfaces repel water spreading
and pore entry. Once dry, replacement of the filter bed is, in most cases, the best
choice in order to avoid poor performance. Hydrophilic surfaces, such as soil,
ceramic or perlite have very low contact angles and (re)wet easily.
3.6 TEMPERATURE
Most biofiltration studies have been carried out under mesophilic conditions, often at
ambient temperature, since many microorganisms are grow under such conditions.
However, waste gas temperatures are very frequently different and most often higher
than temperature ranges corresponding to the optimum activity of mesophilic
microorganisms. On the other hand, in cold regions waste gases may reach
temperature ranges more typical of psychrophilic organisms « 20 aC). It is
sometimes suggestcd that microbial growth rates double with a 10 aC temperature
rise, although this is generally true only in a limited temperature range, since for
temperature increases or decreases of about 20-30 aC above or below the optimal,
growth and substrate biodegradation are very often impossible (Figure 3.10). A
similar trcnd is often observed for biodegradation kinetics as for growth. Biofiltration
at low temperatures has been reported and may be useful in cold regions.
Conventional biofilters operating efficiently at temperatures below 10 ac have been
described, for instance, in the case of H2 S removal (Cho el al., 1992).
Microbial
activity
Psychrophilic Mesophilic Thermophilic
20 40 60
Temperature (0C)
3.7 pH
Here again the addition of buffering agents will allow neutralising the
medium. The addition of chemicals, such as sodium hydroxide for neutralising pH is
not recommended as it might adversely affect the overall removal efficiency through
the accumulation of high salt concentrations and increased ionic strength (Dolfing et
al., 1993).
Contrary to synthetic carriers, some organic filter beds are naturally buffered
and pH fluctuations are reduced to a minimum. In the case of mixed waste gases, the
nature ofthe different pollutants in the air may present a neutralising effect. In a pilot
biofilter treating mixtures of sulphur compounds and ammonia, reaction between
sol- and NH3 allowed maintaining a quite constant pH (Cho et al., 1992).
3.8 PRESSURE DROP AND CLOGGING
Low pressure drop is a common feature of all filter beds during the start-up period.
Problems might show up later and are dependant on many parameters, such as the
nature and characteristics ofthe carrier and biofilm growth.
Pressure drop in packed bed reactors is a well known phenomenon in
chemical engineering. Equations such as the Ergun equation have been used to
Conventional Biojilters 83
quantify it taking into account the major parameters affecting head losses. In packed
bed bioreactors such as gas phase biofilters these parameters include: the nature of
the carrier material, particle size and shape, superficial gas velocity, biomass growth
and water content. In the section dedicated to the different types of carrier materials
used in biofiltration it was already mentioned that synthetic supports generally lead
to lower pressure drops than natural organic ones. A non-uniform flow distribution
and channelling are also more typical of organic carriers than of structured synthetic
ones. The addition ofbulking agents to natural organic carriers allows slowing down
pressure drop increase and optimising flow characteristics in conventional biofilters.
Such compounds include, among others, woods chips, bark, heather, lava particles,
perlite, glass beads or polystyrene. Their effect is shown in Figure 3.11 for compost
and for a compost-perlite mixture. Pressure drop with perlite aloţle was negligible.
Other examples can be found elsewhere (Kennes and Thalasso, 1998). These figures
also illustrate the effect of the gas phase flow rate or superficial gas velocity on
pressure drop. It can easily be observed that at higher gas velocities, head losses will
also increase. The choice of an adequate support is therefore a critical point.
2.5
c. compost
,,-
2
E
2
:;n; 1.5
Q)
I/)D-
I/)~ compost
...
Q)
D- 0.5
+ perlite
O
O 100 200 300 400
30
-
-E 25
ca
-...
C.
.:.:.
C-
o
20
15
"C
...CI>
:::l 10
1/)
1/)
~ 5
c.
O
[A] [B] [C] [O] [E]
Parti ele size range
Figure 3.12. lnfluence of particle size of the filter bed on pressure drop (Yang and Allen,
1994a) (reproduced with permission). Particle size (mm): [A] > 12, [B] = 3.35-12. [el =
2.36-3.35, [D] = 1.18-2.36, [E] < 1.18. Gas velocities (m/h): • = 396,. = 792.
4. Costs
poIlutant concentration may become prohibitive under another set of conditions. One
should also bear in mind that the different technologies are not always suitable for
the same range of waste gas characteristics (see also Figure 2.1). Parameters
affecting operating and capital costs of a given technique might be insignificant for
another one. Recalcitrance to biological degradation which is a key parameter in the
case of biofiltration has no economic al impact on any other non-biologic al technique.
The most significant parameter linked to investment costs in biofiltration is
the price of the filter bed or carrier material. Prices may largely vary from less than
100 Euros / m3 for most natural carriers (soil, compost, wood bark, heather, etc.) to
more than 1000 Euros / m3 for some synthetic or non-natural carriers. Prices may
also slightly vary from one country to another. Some examples are listed below
(orientative prices given in Euros, year 2000):
Price (€)
Compost 40-50/ m3
Heather 100-120/m3
Wood bark 60-75/ m3
Activated carbon 6-9/ kg
Table 3.11. Typical investment and operating costs for different waste gas treatment
technologies
17-105(d) (3)
22.5-67.5(d) (3)
7-140(d) (3)
Conventional Biofilters 87
0.32-0.80 (6)
(Europe)
0.16-0.32
(USA)
(a) fuel costs only, (b) for 0.1-2.0 gvoc/m3 and 10000 m3/h with 50% energy rccovery in
case of incineration and steam regeneration in case of adsorption, (c) for 50000 m 3/h, (d)
concentration dependant, (e) including rege ner. incineration, (f) with regeneration, (g)
chlorine.
(1) Ottengraf and Diks, 1992; (2) Ruddy and Carroll, 1993; (3) van Groenestijn and
Hesselink, 1993; (4) Bohn, 1992; (5) Devinny el al., 1999; (6) Leson and Winer, 1991.
S. Applications
Biofilters have several applications. They may be used for the treatment of industrial
waste gases and for the removal of volatile compounds emitted by waste water
treatment plants. They may also be used in soil and groundwater remediation in
combination with technologies such as soil vapour extraction and air stripping where
contaminants present in a solid phase (soil) or in a liquid phase (aquifers) are
transferred to a gas phase (air). Air pollution generated at composting facilities or
through fugiti ve emissions from storage tanks are other examples of full-scale
biofilter applications.
88 C Kennes and MC Veiga
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CHAPTER 4 BIOTRICKLING FILTERS
1. Introduction
As mentioned in Chapter 3, biotreatment for air pollution control started in the 1950s
using soi! beds. The technology has since matured and industrial applications of
biofilters are numerous. More recent1y research has focused on a variation of
biofilters called biotricklingjilter, or trickling biojilter. Biotrickling filters work in a
similar manner to biofilters, except that an aqueous phase is trickled over the
packing, and that the packing is usually made of some synthetic or inert material,
such as, among others, plastic rings, open pore foam, lava rock. The trickling
solution contains essential inorganic nutrients such as nitrogen, phosphorous,
potassium, etc. and is usually recycled.
Biotrickling filters are more complex than biofilters but are usually more
effective, especially for the treatment of compounds difficult to degrade or
compounds that generate acidic by-products, such as H2S (Oh and Bartha, 1997;
Mpanias and Baltzis, 1998; Cox and Deshusses, 2000b). Biotrickling filters can also
be built taller than biofilters, which reduces their footprint. It is also easier to control
the conditions because ofthe free liquid phase, so that difficult applications are better
handled by a biotrickling filter than by a biofilter. These include but are not limited
to the treatment of high concentrations of contaminants, treatment of hot gases and/or
of acid producing contaminants, treatment of air streams containing grease or
particles, etc. Biotrickling filters are more recent than biofilters. and have not yet
been fully deployed in industrial applications, but the prospective future applications
are promising. The advantages and disadvantages of biofiltration and biotrickling
filtration are compared to those of conventional air pollution control techniques in
Table 4.1.
The basic mechanisms of biotrickling filtration are shown in Figures 4.1 and 4.2.
Contaminated air is passed co- or counter-current1y through a packed bed of inert
materials on which a pollutant-degrading biofilm has established. At this time, there
is no clear agreement as to whether co-current or counter-current is better.
Mathematical modelling of kinetically limited systems (Diks and Ottengraf, 1991 b,
Zuber, 1995) suggests that co-current is better, since it minimises stripping near the
air exit, but experiments have failed to demonstrate that this was indeed true. For
mass transfer limited systems, the flow direction may not mat1er (Lobo el al., 1999).
Constraints specific to the equipment construction might prevail until further
demonstration that one or the other operating mode is preferred.
99
C. Kennes and M. C. Veiga (eds.), Bioreactorsfor Waste Gas Treatment, 99-131.
© 2001 Kluwer Academic Publishers.
100 HHJ Cox and MA. Deshusses
Table 4.1. Comparison of biofiltration, biotrickling filtration and conventional air pollution
control techniques
Illlct air
(contamillatcd)
Figure 4.1. Schematic ofbiotrickling filter set up (co-current and forced draft shown).
il
Pollutanl End Product
H~drocarbon CO, - H,O
H,S --. '0, '
Reduced ""Ifur 0;- + CO.
NO." I-CO.)
Pollul anl (. ,1 •
The feed rate and nutrient concentration is based on the expected nutrient
requirements of the process culture. Based on typical growth media recipes,
biotrick!ing filters often receive less nutrients than stoichiometrically required. This
is because the nutrients are internally recycled by cell death, endogenous biomass
digestion, and predators such as protozoa and rotifers. Nutrient !imitation can also be
a deliberate choice of the operator, in an attempt to limit bacterial growth and slow
down biomass accumulation, as discussed in Section 5.5. Interestingly, the nutrient
deficiency can be as high as a factor 20 of the theoretical amount required without
severe consequences as far as pol\utant removal rates are concerned. The
determination ofthe feed rate and feed composition should also consider keeping the
concentration of any salt or metabolite below any possible inhibitory concentration,
although as wil\ be discussed in Section 5.5, some investigators have on purpose
al\owed the salt concentrat ion to rise, again, in an attempt to !imit biomass growth.
102 HHJ Cox and MA. Deshusses
Biotrickling filters differ from biofilters in that there is a free liquid phase. In
most cases the trickling solution is recyc1ed, although in a few application with very
low trickling, a one pass of the liquid has been used. Overall, a wide variety of
conditions have been experienced for trickling rates usually ranging from 0.05 to 20
m/h. The trickling rate influences the wetting of the packing and therefore the mass
transfer ofthe pollutants to the biofilm. The trickling rate also influences the pressure
drop over the packed bed. The fact that biotrickling filters work with only partial
wetting of the biofilm, suggests that pollutants can transfer from the gas to the
biofilm directly, or they can transfer from the gas to the trickling liquid, and then to
the biofilm. While the latter path is generally assumed, mechanisms and rates for the
direct transfer from the gas to the biofilm has been vastly ignored (Cox and
Deshusses, 1998).
As far a pollutant degradation is concemed, most ofthe degradation occurs in
the biofilm, although in selected cases, significant activity can occur in the recyc1e
liquid, as reported by Cox el al. (2000). Examination of Figure 4.2 reveals that
pollutant elimination is the result of a complex combination of mass transfer
(diffusion, convection) and biological processes, such as growth, death and lysis,
predation. These are complicated by the fact that the biofilm houses multiple species
in a complex architecture. All ofthese are affected by the operating conditions ofthe
system and also affect the pollutant removal and the general dynamic of the
biotrickling filter. Under these circumstances a complete description of ali the
phenomena involved in a biotrickling filter is not yet available. While an improved
fundamental understanding would be desirable for re actor design and operation, the
lack of fundamental understanding does not prevent application ofthe technology.
.
Remova l EffilClency = RE = C m - C OU!
100 (%) (4.1)
C in
V (4.3)
Empty Bed Retention Time = EBRT = Q (s or min)
where Cn and Cout are the inlet and outlet pollutant concentrations (usually in g/m3 or
in dilution to threshold for odour removal), respectively, V is the volume of the
packed bed (m3) and Q is the air flow rate (m 3/h). Pollutant concentrations are
usually reported as mass per volume; conversion of volumetric to mass
concentrations (C) is done using the ideal gas law which reduces to Equations 1.1 or
1.2 recalled below for room temperature conditions (see Chapter 1):
It should be stressed that the elimination capacity and the loading are
calculated using the volume of the packed bed and not to the total volume of the
reactor. Depending on the reactor design, the volume of the packed bed volume will
be about 40-90% of the total reactor volume. Aiso the EBRT is calculated on the
basis of the total volume of packed bed (Equation 4.3) and not the void space in the
packing. The actual gas residence time wi\l be lower depending on the porosity of the
packing, the dynamic liquid hold-up and the amount of biomass attached to the
packing. The porosity of packing ranges from about 50% (lava rock) to 95% (ali
random or structured packings), the liquid hold-up is usually less than 5% ofthe bed
volume, and biomass may occupy 5% to 30% of the bed volume. Hence, the actual
gas residence can be less than halfthe EBRT.
A typical elimination capacity vs. pollutant loading curve is shown in Figure
4.3. Note that it is similar to curves obtained for conventional biofilters. It is usual to
report the performance as a function of the load, i.e., inlet concentration x air flow.
rather than the concentration. This enables comparison of systems of different sizes
operated under different conditions. One underlying assumption is that the
performance depends only on the pollutant load, hence, that low concentrations-high
flowrates conditions lead to similar elimination capacities than high concentrations-
low flowrates. This assumption is generally valid because the pollutant
concentrations commonly encountered in biotrickling filters are often high enough
for the micro-kinetic to be of zero order. As schematically shown in Figure 4.3, this
is no longer true at very low pollutant concentrations (typically below 0.05-0.1
g/m 3), in particular for pollutants with high Henry's law coefficients, because first
order kinetics will prevail in the biofilm resulting in a reduction of the maximum
elimination capacity.
190% removalline
Figure 4.3. Schematic of a typical elimination capacity VS. (oad curve for a biotrickling
fiIter.
104 HHJ Cox and MA. Deshusses
Examination of Figure 4.3 reveals that there are essentially three operating
regimes, as for the case of conventional biofilters:
1. Low loading, also called first order regime. The elimination capacity and the
loading are identical and the pollutant is completely removed. The biotrickling
filter is operated well be10w its maximum e1imination capacity. The performance
increases proportionally with the loading.
2. Intermediate range. Breakthrough of the pollutant occurs. With higher inlet
concentrations or higher air flow rates, the e1imination capacity increases, but to
a lesser extent than the loading.
3. High loading, also called zero order regime. The biotrickling filter is operated at
its maximum elimination capacity. Increases in loading do not result in further
increases in elimination capacity, the removal efficiency decreases. As indicated
on the figure, if the concentration is very low, the maximum elimination capacity
is reduced accordingly.
For the evaluation ofbiotrickling filter performance, one should consider both
the maximum elimination capacity and the removal efficiency. For practical reasons
academic research is mainly concemed with the maximum elimination capacity OI
with high performance, which occur at relatively high pollutant concentration and
often less than -90% removal efficiency. On the other hand, reactor design for
industrial application often needs to meet a certain discharge requirement, or achieve
a high removal percentage. Thus there might be some chaUenges in extrapolating
research data for reactor design.
control routines using logic statements to detect abnormal operation, and propose or
implement remedial action via feedback controllers (Webster et al., 1999). For
instance, the medium feed and purge might be controlled using the input of
conductivity probe (as an indicator of the overall salt concentration) installed in the
recycle liquid, and the input of a level switch. However, it should be stressed
sophisticated controls are not always necessary. The low tech alternative for the
above will consider an operator removing a given volume of the recycle liquid on a
given schedule (daily or weekly) and replace it with water and a mineral nutrient
mix, often fertiliser grade. The choice of sophisticated controlor mostly manual
operation depends on the application, the size of the reactor, the regulatory agency
and the available budget.
Monitoring the re actor performance is often defined in the permitting of the
biotrickling filter. It can be on-line integrated with the process control, or off-line by
grab samples. Monitoring is an important part of operation and maintenance. Proper
monitoring helps in troubleshooting and in optimising the operation of the reactor.
Most important is the monitoring of pollutant removal. For VOCs this is best done
using a flame ionisation detector, while for H2 S, and ammonia, special meters are
available. Monitoring tubes can also be conveniently utilised. For odour treatment,
odour panels are still the best measurement although they are expensive. The
measure of the odour removal efficiency is usually based on the odour dilution-to-
threshold, although the character of the odour should also be considered. Inlet and
outlet should always be measured. The frequency of the measurement depends on the
regulatory requirement, the equipment used and the operating conditions of the
biotrickling filter (steady conditions or rapid transients).
Other parameters to consider in a monitoring plan include airflow rate,
reactor temperature, pressure drop, biomass content, and parameters pertaining to the
recycle liquid, such as flow rate, pH, ionic strength, biological oxygen demand, and
possibly dissolved oxygen in the case of the treatment of high pollutant
concentrations. Structural inspection and proper functioning of the biotrickling filter
components (e.g., spray nozzles, feed lines, etc.) are also important. The challenge of
defining a good monitoring plan will be to schedule the necessary sampling that
allows for a good control of the biotrickling filter and an early detection of possible
problems, while minimising maintenance and analytical costs.
Over the past decade, many pollutants have been tested for treatment in biotrickling
filters, mostly in the laboratory. Effective removal has been reported for aliphatic and
aromatic hydrocarbons, oxygenated hydrocarbons, chlorinated hydrocarbons and
inorganic compounds. Typical examples are presented in Table 4.2. Most pollutants
contain carbon and they serve as a carbon and energy source for aerobic,
heterotrophic microorganisms. Other biological processes observed Of applied in
biotrickling filters include:
species are in general autotrophic, using carbon dioxide from air as the carbon
source for growth. Another example is the oxidation of ammonia to nitrate.
Effective removal of ammonia in a nitrifying biotrickling filter has been
demonstrated by van Groenestijn and Lake (1999). In a second denitrification
reactor, the produced nitrate was reduced to nitrogen gas as the final product of
the combined system.
• Co-metabolism. An example is the removal of trichloroethylene in biotrickling
filters (Sun et al., 1998). Cometabolism requires the presence of an inducing
growth substrate, which may be already present in the waste gas or has to be
added artificially.
• Anaerobic removal of compounds that are persistent under aerobic conditions
(Section 4.2).
performance is very reproducible provided that the reactors are operated under
identical conditions. In a comparative study with twenty identical, toluene-degrading
biotrickling filters operated in parallel, the average maximum elimination capacity
was 79 g/m 3 .h with a standard deviation of 5.7 g/m 3 .h (Cox and Deshusses, 2000a).
~
u 200
ro
o..
ro
u
C 150
.Q ~
....,
ro . ~
C(Y)
E __
.- E 100
=<1l~
OJ
E 50
:::J
E
'xro
O
~
+ ++ +++
Biodegradability of pollutant
Figure 4.4. Maximum elimination capacities averaged for pollutants grouped by increasing
biodegradability.
Aromatie hydrocarbons
Styrene ++ 0.11 15 days 32 Pol el al, 1998
Styrene' ++ 0.11 NA 35 Webster et al, 1999
Toluene +++ 0.28 10 days 80 Cox and Deshusses, 1999'
Oxygenated hydrocarbons
Propionaldehyde +++ 0.0024 NA 300 Kirchner et al., 1992
Acetone +++ ~
0.0016 NA 500 Kirchner et al., 1992
Methyl ethylketone +++ 0.0024 NA 40 Chou and Huang, 1997
o'
'::;'
Methanol +++ 0.00019 5 days 100 Allen el al., 2000 ;::;.
n-butanol +++ 0.00035 NA 100 Heinze and Friedrich, 1997 i:t
S·
Diethyl ether + 0.028 2 weeks 60 Zhu el al., 1996 (Jq
Methyl-tert-butyl ether + 0.023 7 months 45 Fortin and Deshusses, 1999 ~
::;:-
Chlorinated hydrocarbons ;:;'"
Dichloromethane +++ 0.093 1 week 200 Hartmans and Tramper, 1991
+++ 0.093 1 week 157 Diks and Ottengraf, 1991 b
Chlorobenzenes ++ 0.18 NA 300 Ob and Bartha, 1994
++ 0.18 NA 60 Mpanias and Baltzis, 1998
Parameter Pedersen and Arvin, Cox and Deshusses, Smith et al., Schiinduve et al., Weber and Hartmans,
1995 1999a 1996 1996 1996
Reactor design
Reactor, lD x H (cm) 9x70 15xl30 15x114 15x25 30xlO0
Packing Steel Pall rings PP Pall rings Celite pellets PP Pali rings Pall rings ;::r::
Specific surface area (m 2/m 3 ) 317 220 1190 NA 110 ;::r::
Inoculation Adapted consortium Pseudomonas Sample of reactor Adapted consortium Bacterial Fungal '-..
corrugata consortium consortium
Q
Reactor operation ~
"
;:s
Gas flow Upflow Downflow Downflow Upflow Upflow \:)..
Empty bed gas residence time (5) 32-160 56 60-120 17-132 36
~
Toluene inlet concentration (glm 3 ) 0.19-1.61 0.5-3.5 0.93 0.2-3.8 0.7 ~
Superficial liquid velocity (m/h) 3.3-4.7 7.9 0.05 22.6 1.6
Continuous Semi-continuous' Batch Batch
O
ti)
Nutrient feed Batch
Nutrient composition Semi-full medium Full medium Full medium Full medium Full medium Complete, limiting ;::-
'"
;:::
N-NH/ N-N0 3' concentrations
ti)
'"'"
Liquid residence time (day) NA 0.5 NA NA
'"
Reactor performance
Load (g/m 3 h) 6-150 35-225 60 -50-1300 70
Elimination capacity (g/m 3 .hl 35 71-83 60 120 33 18 34
'No liquid recycling, but once-through pass of fresh medium.
Biotrickling filters 111
Although biotrickling filter research in the US has trailed Europe over the past two
decades, recently rapid progress has been made especially in the area of odour
control at waste water treatment facilities. Waste gases at these facilities contain
hydrogen sulphide (H2S) as the principal odour causing agent in concentrations up to
100 ppmv as well as lower concentrations (0-100 ppbv) of various VOCs and
chlorinated hydrocarbons. Chemical scrubbers are currently employed to reduce the
odour problem. Although they are effective in removing H2S, the high consumption
of chemicals (caustic soda, hypochlorite) and their ineffectiveness in controlling
VOCs are drawbacks of increasing concern. Demonstration projects, many of them
located in Southern California and conducted by universities, waste water treatment
facilities and industry, focus on using biofilters and biotrickling filters as alternatives
for chemical scrubbers.
In 1993, a biotrickling filter study was done at the Los Angeles County
Sanitation Districts (Morton and Caballero, 1996). Greater than 98% and 99%
removal of respectively H2S and odour was demonstrated in a pilot unit of 0.3 m3
with lava rock as the packing material. The gas residence time was varied between
12 and 30 seconds, which is considerably more than the typical detention time in
chemical scrubbers (2-5 s). A constant pH of 2.0-3.0 was maintained by
continuously supplying secondary effluent water and purging the produced sulphuric
acid. The secondary effluent water also proved to be good source of nutrients for
growth and activity of H2S oxidising bacteria. Because of concerns of clogging of the
lava rock, a second experiment was set up using a porous plastic p.acking. The H2S
removal efficiency was lower, presumably because of mass transfer limitation due to
a lower specific surface area of the packing. The study of Morton and Caballero
(1996) illustrates the importance of packing material selection.
Co-treatment ofH2S and VOCs has been studied in a number ofprojects. For
optimisation of both removals, there may be a conflict of pH optima. H2S is in
general oxidised by Thiobacillus species with an optimum pH of about 2. VOCs are
degraded by heterotrophs that generally prefer a neutral pH, although VOC removal
in low pH, H2S oxidizing biofilters and biotrickling filters has been observed (Torres
and Basrai, 1998; Chitwood el al., 1999; Cox and Deshusses, 2000b). Chitwood el
al., 1999 investigated a two-stage process at the Ojai Valley Sanitary District. This
process consisted of an acidic reactor with lava rocks for H2S removal, followed by a
pH-neutral biofilter for VOC removal. The acidic reactor had a very low intermittent
trickling rate. Overall performance and removal efficiency of the two stage process
seemed slightly better than combined removal in a single stage biofilter (Chitwood el
al., 1999). Other studies have focused on biotrickling filters operated at a neutral pH
by automated caustic soda addition, for simultaneous removal of H2S and VOCs. A
pilot-scale biotrickling filter at the County Sanitation Districs of Orange County
removed greater than 87% of H2S but removal of VOCs was disappointingly low at
11 % (Torres and Basrai, 1998). Low VOC loadings and frequent systems upsets
were the presumed causes for poor VOC removal. Nevertheless, this study shows the
potential of pH-neutral biotrickling filters for the simultaneous removal of H2S and
VOCs.
112 HHJ Cox and MA. Deshusses
4.1 TEMPERATURE
4.20XYGEN
Figure 4.5. Schematic representation of oxygen and pollutant concentration profiles in the
biofilm.
(4.6)
where D02 and Dpoll are the diffusion coefficients of oxygen and of the pollutant in
the biofilm, C02 ,i and Cpoll,i are the concentrations of respectively oxygen and the
pollutant at the biofilm interface, while the ratio Vpo ll/V02 (mg pollutant/mg oxygen)
reflects the reaction stoichiometry. Oxygen limitation will occur when A < 1,
114 HHJ Cox and MA. Deshusses
Many different sorts of packing materials have been tested in biotrickling filters.
Important requirements to the packing include a large specific area, high porosity,
high chemi cal stability and structural strength, low weight, suitable surface for
bacterial attachment and growth, and low cost.
A commonly used packing material is lava rock (e.g., Morton and Caballero,
1996; Fortin and Deshusses, 1999). This material has the advantage of providing a
large specific surface, a porous structure that facilitatcs colonisation by
microorganisms (Fortin and Deshusses, 1999). and a low price. Disadvantages are
the low porosity (-50%) and the heavy weight which requires special construction of
the reactor. Another disadvantage we recently observed in the laboratory is that lava
rock is not chemically inert. A substantial weight loss was observed over several
months at a low pH. This might be of importance for biotrickling filter applications
with a low pH, e.g., odour treatment and H2S removal at waste water purification
plants as discussed in Section 3.3.
Random dump plastic packings such as Pall rings have bccn used in many
laboratory studies and large scale reactors. These packings are casy to handle.
however, experiments indicate that start-up is relatively long presumably because
Biolricklingfilters 115
poor biofilm establishment on the surface (Fortin and Deshusses, 1999; Kazenski and
Kinney, 2000). AIso, the relatively low specific surface area is a disadvantage for
achieving a high elimination capacity (Webster el al., 1999). On the other hand, the
use of plastic packing may be beneficial because of its stability, low cost and high
porosity (Kazenski and Kinney, 2000). Structured packings made from stainless steel
or plastic combine a high porosity and large specific surface. Good performance has
been observed with these type of packings (Zuber, 1995; Webster et al., 1998), but
they are more expensive.
Activated carbon-based packings have adsorbing properties that are not
encountered in other materials. It is often assumed that adsorption is beneficial
especially when the pollutant concentration in the waste gas is fluctuating ('peak
dampening'). However, activated carbon particles in biotrickling filters will bc
covered by a biofilm, which will decrease the absorptive capacity of the carbon. A
better option would be using a separate activated carbon unit preceding the
biotrickling filter (Weber and Hartmans, 1995).
A relatively new packing used in biotrickling filters is open-pore
polyurethane foam products. Published data on the performance are scarce, but some
major European vendors offer these products, often for biotrickling filters designed
for H2S removal. Our own experiences in the laboratory (unpublished) indicated
improved performance with polyurethane foam cubes over other types of packing,
especially at high gas flow rates with low H2S concentrations. Owing to the open
structure and high porosity, the pressure drop over the packing remained low at a
relatively high gas velocity. The large specific surface area proved beneficial with
respect to mass transfer limitation observed at low H2S concentration.
Activated sludge
High Low
Soillwater sample from
contaminated site
1.2
1.0
0.2
0.0
O 50 100 150 200 250 300
Time (days)
Figure 4.7. Start-up ofMTBE degrading biotrickling filters inoculated with different sources
of microorganisms (Cox and Deshusses, unpublished data for the pure culture and adapted
consortium, Fortin and Deshusses, 1999 for the contaminated soil and water inoculum data).
4.5 NUTRIENTS
Pollutant - C
Air/water - - O, H - - - 1 - +
Medium - N, S, P, K, Mg
~ Trace elements
Fe, Cu, Mo, etc.
Figure 4.8. Utilisation of nutrients by heterotrophic bacteria with the pollutant as the carbon
source for growth.
ca1culations it is assumed that the waste gas pollutant is the carbon source for
microbial growth. Since the pollutant is the limiting substrate, the amount of biomass
formed is proportional to the amount of pollutant degraded. The first step is to
calculate the expected biomass accumulation rate (X,ee in g dry biomass/m3 reactor.
h) from the desired or design value for the e1imination capacity (g C-pollutant/m3
reactor.h) and the biomass to carbon yield coefficient (g dry biomass/g carbon):
(4.8)
where YXIE is the biomass yie1d coefficient on element E (g dry biomass/g element
E). Typical examples of biomass yield coefficients are listed in Table 4.4. Note that
these are for pure cultures growing in bioreactors, recommended values for
biotrickling filtration are probably close to those listed as the upper limit.
The above calculation assumes that nutrients supplied are irreversibly
incorporated into a continuously growing primary culture. Cell death and Iysis, and
the presence of a secondary population and predators in the biotrickling filter is thus
neglected. These processes result in nutrient-recycling, causing a larger availability
of nutrients. The supply rate of nutrients can be decreased accordingly, but this is
very difficult to quantify. Experiments with toluene degrading biotrickling filters
have indicated that nutrient recycling by secondary processes may reduce the
required nutrient supply rate by a factor two (Cox and Deshusses, 2000c). Not
unexpectedly, the recycle of nutrients by predation and secondary processes is
Biotrickling filters 119
irrelevant when excess nutrient is provided. Under these circumstances rapid growth
of biomass and re actor clogging is often experienced. This is further discussed in
Section 5.
For full-scale biotrickling filters it is often not practical or too expensive to
feed a chemically defined medium. Alternative nutrient sources include agricultural
fertilisers and secondary effluent water from waste water treatment plants. Although
these sources may not have the most ideal composition, they have shown to be
satisfactory in supporting sustained pollutant elimination in pilot-scale biotrickling
filters (Webster et al., 1999).
A distinctive feature of biotrickling filters is the recycling of a liquid phase over the
packing. The recycle liquid supplies water and nutrients to the biofilm and it removes
metabolic products that would otherwise accumulate in the biofilm in possibly toxic
concentrations. Continuous monitoring and adjustment of chemi cal parameters in the
recycle liquid allow for better control of microbial activity in the biofilm, which is an
important advantage ofbiotrickling filters over biofilters.
Biotrickling filters can be operated with the gas and liquid flowing co-
currently or counter-currently. Co-current operation is often advocated, as counter-
current operation would allow stripping of the pollutant from the liquid phase at the
gas outlet side of the re actor, thereby causing a lower elimination capacity. This is
merely a matter of theoretical concern. Experimental data indicate no major
difference between either mode of operation (Diks and Ottengraf, 1991b). Moreover,
stripping effects are likely to occur only in biotrickling filters overloaded with the
pollutant, causing a high pollutant concentration in the liquid phase. In most field
applications a near complete removal of the pollutant is usually the objective, in
which case the pollutant concentration in the liquid phase will be negligible as well
as possible stripping effects.
The rate of liquid recycling is often expressed as the superficial liquid
ve1ocity. Ve10cities typically range from 0.05 up to 20 m/h. Usually an increase of
the elimination capacity is observed with a higher superficial liquid velocity. This
has been attributed to an increase of the wetted biofilm surface area (Diks and
Ottengraf, 1991 b), or to a reduction of mass transfer resistance in the liquid phase
(Hartmans and Tramper, 1991). Treatment of pollutants that release acid end-
products is a case that requires special attention. At too Iowa trickle rate, the liquid
may not be able to remove the produced acids fast enough so that the pH could be
120 HHJ Cox and MA. Deshusses
reduced to the extent of inhibiting microbi al activity (Diks and Ottengraf, 1991 b; Oh
and Bartha, 1994). This situation can be assessed by caiculating the expected pH at
the bottom of the column using the trickle rate, the acid production rate and the
trickling liquid buffer capacity. Altematively, one could measure the pH in the liquid
trickling from the bottom of the packed bed.
The upper !imit of the superficial liquid velocity is determined by the
flooding point of the reactor, which will de crease over time as biomass accumulates.
The superficial velocity will also have an effect on the removal of hydrophobic
pollutants. Thick layers of recycle liquid covering the biofilm may act as a barrier,
causing a reduced mass transfer rate of the pollutant from the gas phase into the
biofilm (Zhu el al., 1998; Nascimento el al., 2000). This type of mass transfer
resistance can be reduced by lowering the superficial liquid velocity. Also
intermittent instead of continuous liquid recycling may improve the mass transfer of
hydrophobic pollutants and improve their removal in biotrickling filters (Wolff,
1992; Pol el al., 1998).
With continuous supply of nutrients, the biotrickling filter will accumulate large
amounts of biomass. At present, clogging of thc re actor over the long run is one of
the major obstacles at the industrial scale. This section describes the various stages of
biomass accumulation, the consequences for the performance and long-term stabi!ity,
and methods to control biomass growth.
In general, pollutants are used by the primary culture to produce new biomass and to
generate energy for maintenance activities of the existing biomass. The biotrickling
filter process can at first instance be considered as a continuous culture (e.g.,
neglecting secondary processes, local heterogeneities, and mass transfer effects):
EC = (1l1Y + m) X (4.9)
).Ima, S (4.10)
).1
Ks + S
via the liquid purge each sub-population present in the system. This is shown in
Equation 4.11, which expresses the overall biomass accumulation rate in the
biotrickling filter as the sum of accumulation rates of sub-populations (e.g., primary
culture, secondary population, predators) present in the biotrickling filter.
where d is the specific death rate of the sub-population. Predation and wash-out of
biomass have received little attention in biotrickling filter research and these
processes have not been quantitatively described as yet. Despite the limitation of
being virtually impossible to solve, Equation 4.11 demonstrates that the overall
biomass accumulation rate in biotrickling filters depends on the intrinsic microbial
growth rate on the one hand, and various mechanisms of biomass reduction on the
other hand. This allows for development of various strategies to control the
accumulation ofbiomass, as discussed in Section 5.5.
Biotrickling filters are often operated with sufficient supply of nutrients to maximise
the pollutant removal rate. Various stages of biomass accumulation can be
distinguished after inoculation of the biotrickling filter with an appropriate source of
microorganisms. At first, a lag phase will occur during which the microorganisms
adapt to environmental conditions in the reactor and to the pollutant (Figure 4.9). The
duration of the lag phase mainly depends on the biodegradability of the pollutant.
Lag phases as short as a few hours to a few days have been reported for e.g. ethanol
and toluene. On the other hand, removal of methyl-terl-butyl ether (MTBE), a
gasoline additive with low biodegradability, may only be observed after several
months of operation (see Section 4.4).
The exponential growth phase follows the lag phase (Figure 4.9), with rapid
biomass accumulation and an exponentially increasing biofilm thickness (Pedersen el
al., 1997). Pollutant degradation takes place throughout the entire biofilm and the
overall pollutant removal rate increases with the thickness. During this phase a short
term peak in the elimination capacity can sometimes be observed. This has been
linked to a rapid proliferation of suspended biomass in the recyc1e liquid (Cox et al.,
2000). Generally, the. pollutant removal rate soon reaches a constant value (Figure
4.9, pseudo steady state). At this point, diffusion limitation ofthe pollutant (Okkerse
et al., 1999), oxygen (Kirchner el al., 1996; Mpanias and Baltzis, 1998) and/or
nutrients (Zhu el al., 1996; Rihn el al., 1997) in the biofilm causes biodegradation to
take place only in the upper layer at the gas/biofilm interface. Similar to fixed film
waste water treatment processes, the effective biofilm thickness in biotrickling filters
is as a rule of thumb in the order of 25-300 Ilm (e.g., Kirchner el al., 1996;
Schonduve el al., 1996; Mirpuri et al., 1997a).
Prolonged operation with nutrient supply causes further growth of the
biofilm, however, the effective biofilm thickness and the elimination capacity remain
constant (Zuber, 1995; Cox and Deshusses, 1999a; Okkerse el al., 1999). Prolonged
operation therefore primarily results in formation of biomass not actively involved in
biodegradation. Thick biofilms in biotrickling filters contain large fractions of
inactive or dead cells and inert material (Schonduve el al., 1996; Hugler et al., 1996;
122 HHJ Cox and MA. Deshusses
Effective biofilm
Diffusion limited
Inactive
Time
Figure 4.9. Schematic of the long-term performance of biotrickling filters with continuous
supply of nutrients. The upper section shows the development of the elimination capacity
over time, whereas biofilm grown is shown in the lower section. (Note that the schematic is
not to scale).
Okkerse et al., 1999; Pedersen et al., 1997). Finally, biotrickling filters subject to
excessive biomass formation (Figure 4.9, clogging) face c10gging with increasing
pressure drops across the reactor and a decreasing pollutant removal rate (Cox et al.,
1998; Cox and Deshusses, 1999a; Okkerse el al., 1999).
showed that the mass transfer coefficient (KLa) in biotrickling filters was 25-140 %
larger when the packing was covered by a biofilm.
Table 4.5. Example ofthe estimation ofthe biomass accumulation rate in biotrickling filters
treating toluene vapours. The amount of biomass produced in 77 days is equal to the total
reactor volume
The first option to prevent clogging is reduction of the biomass accumulation rate
(Equation 4.11). According to Equations 4.9 and 4.11, this can be achieved by
reducing thc biomass yield coefficient (Y XlS), by increasing the maintenance
requirements (m s) or by stimulating predation or the death rate. The challenge is to
maintain a high pollutant removal rate (Equation 4.9), however, growth, yield,
activity and maintenance are interrelated parameters reflecting general cell
metabolism and, as such, they are often difficult to influence independently.
Various strategies to reduce the specific growth rate in biotrickling filters
have been investigated in the laboratory (Table 4.6). These include limiting the
supply of nutrients essential for growth, the use of nitrate as a nitrogen source instead
of ammonium and the addition of compounds such as NaCI in concentrations that
partiaIly inhibit microbial growth. In general, these strategies also result in reduction
of microbial activity. Hence, a relatively large re actor volume will be required to
treat the same volume of waste gas at the same efficiency. An interesting option is
the use of fungi, as these types of microorganisms show a higher removal rate than
bacteria under nutrient-limiting conditions in toluene degrading biotrickling filters
(Weber and Hartmans, 1996). Predation of biomass by higher organisms such as
protozoa is a relatively unexplored area in biotrickling filter research, although the
phenomenon is quite known in waste water treatment systems. Protozoa are natural
inhabitants of bioirickling filters, and stimulation of their activity was showed ta
reduce the biomass accumulation rate (Cox and Deshusses, 1999a). The advantage of
predation over options mentioned earlier is that the process culture is allowed to
grow at the maximum rate, and hence with maximum microbi al activity. In fact,
stimulation of pratozoan predation caused a slight increase of the maximum
elimination capacity, which was tentatively attributed ta an increased rate of nutrient
recycling (Cox and Deshusses, 1999a). The predation rate was, however, not high
enough to fully counterbalance micrabial growth, and only delaying clogging of the
reactor could be achieved.
The second option to prevent clogging is periodical removal of the produced
biomass. In this scenario the biotrickling filter is operated at a high climination
capacity allowing rapid accumulation of biomass. Removal of biomass can be done
physically or chemically (Table 4.6). Physical removal of biomass relies on biofilm
detachment by high shear forces. This can be do ne by backwashing of the reactor, or
by periodical stirring of the packed bed. Although these techniques result in
prolonged, stable biotrickling filter operation, certain drawbacks exist (Table 4.6). It
should be noted that shear stress of the trickling liquid during normal operation of the
biotrickling filter is not sufficient to remove substantial amounts of attached biomass
(Pedersen et al., 1997; Cox and Deshusses, 1999b). Chcmical removal of biomass is
a simple operation as no major changes of the reactor configuration are required. A
stable toluene degrading biotrickling filter has been obtained by periodical washing
of the packing with a NaOH solution for 3 hours (Weber and Hartmans, 1996). A
post-treatment with HCI was needed to restore the pH to a neutral value. Other
chemicals such as sodium hypochlorite and hydrogen peroxide may be more
effective in removing biomass, but they are also more toxic to the micrabial
population (Cox and Deshusses, 1999b). This could potentiaIly slow down the restart
ofthe reactor.
Table 4.6. Control ofbiomass accumulation in biotrickling filters
6. ConcIusions
Biological waste water treatment has become part of our everyday life. Although, the
process is not fully understood, waste water treatment is a major improvement for
water quality. More than 100 years after the introduction of the first waste water
treatment plants, bioreactors for the treatment of gaseous effluents have the potential
to play a similar role for air quality. In the past decades major progress has been
accomplished in the development of vapour-phase bioreactors, in particular in
biotrickling filters. While the level of understanding of the biotrickling filtration
process sti Il remains limited, the evident success of waste water biotreatment should
be a motivation to pursue active research. Clearly, thc full potential of biotrickling
filtration for air pollution control has not yet been explored. There is great promise
for both effective and environmentally friendly biotreatment of contaminated gases.
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CHAPTER 5 BIOSCRUBBERS
1. Introduction
The last two points are also advantages compared to bio-trickling filters.
Disadvantages:
• Only cost-effective for pollutants with a dimensionless Henry's law's coefficient
be10w 0.01;
• More difficult to attain elimination efficiencies higher than 98%;
• Chance ofthe slowest-growing micro-organisms being washed out;
• Stagnation periods of some days are not permitted;
• Disposal of sludge;
• More complicated start-up procedure;
• Higher operational costs.
133
C. Keflfles afld M. C. Veiga (eds.), Bioreactorsfor Waste Gas Treatmeflt, 133-162.
© 2001 Kluwer Academic Publishers.
134 J W van Groenestijn
Packed bed
Water
level
sensor
0---:
o - o
o o o
Absorber o o o o o o o
o o
o o o o
Fresh waler o
Waste
Tilranl -------(:t----t.,-~~__:::_:-___:-~~J------'--~-- waler
Nutrienl
solulion
Blower
Figure 5.1. Bioscrubbcr (the waste gas is introduced in the absorber in which the pollutants
are transferred to the water phase, subsequently the water is transferred to the bioreactor in
which the pollutants are biodegraded).
2. Absorbers
2.1 CONSTRUCTION
The primary function of the gas absorption contactor is to provide an extensive area
of liquid surface in contact with the gas phase under conditions favouring mass
Bioscrubbers 135
transfer (see also Chapter 2). Contactors normally employ at least one of the
foIlowing mechanisms: (1) dividing the gas into small bubbles in a continuous liquid
phase (e.g., bubble cap trays) , (2) spreading the liquid into thin films that flow
through a continuous gas phase (e.g., packed columns), and (3) forming the liquid
into smalI drops in a continuous gas phase (e.g., spray chambers) (Kohl and Nielsen,
1997).
For bioscrubbing, the packed towers are recommended, as the other types
show poor elimination efficiencies for compounds relatively poorly soluble in water,
i.e. with dimensionless Henry's law coefficients near 0.01. Venturi scrubbers are best
in entrainment of small mist drops « 10 ~m), fumes « 1 ~m) and fine dust (l-S
~m), but weak in transfer of volatile compounds. In Table 5.1 typical gas velocities
and pressure drops for scrubbers can be found. The low pressure drops in counter-
current packed contactors are appreciated in industry, because of the lower energy
costs connected, despite of the larger volumes compared with co-current packed
contactors. Co-current operation aIlows the use of very high velocities without
concern of flooding. However, the gas velocities which are possible in co-current
packed absorbers are seldom required in bioscrubbing. Moreover, the absorption
efficiencies of co-current absorbers are lower than that of counter-current absorbers,
as in the latter the elean gas is contacted with the elean (also called 'Iean') water.
Cross flow operation of packed absorption towers is characterised by a horizontal
flow of the gas and a vertical flow of the water. However, the water wiIl not move
perfectly verticaIly, but with a slope, because of the horizontal forces of the flowing
gas. Therefore, it is recommended to use packed beds shaped with a slope
(parallelogram).
For bioscrubbers counter-current packed towers are recommended. The
towers comprise the folIowing elements (from bottom to top): a liquid reservoir or
sump, a gas inlet (generalIy one large opening), a packed bed, a space with spray
nozzles or other liquid distribution devices, a demister and a gas oudet. The packed
bed is mostly filIed with special low pressure, high efficiency plastic packing.
Examples are Jaeger Tri-packs (Jaeger Products Inc.), Intalox Snowflake packing
(Norton Chemical Process Products Corp.), TeUerettes (Ceilcote Air PoUution
Control) and Maspac (Clarkson Controls and Equipment Co.) (Kohl and Nielsen,
1997). These are randomly placed materials. Conventional random packing materials
are Raschig and PaU rings and saddles. Recently, structured packing materials gain
more popularity. The packing materials mostly have specific surface areas between
136 1. W van Groenestijn
100-300 m 2/m 3 (Fischer,1990), but not al! parts of the surface may be wetted aII the
time (2/3 of the total surface seems realistic). The sizes of packing elements range
from 2 to 8 cm. Kohl and Nielsen (1997) recommend a ratio of the diameter of the
column and the packing elements of at least 15: 1. Because of the deformability,
plastic packing is limited to an unsupported height of 3 to 5 m.
Table 5.1. Typical gas velocities and pressure drops for wet scrubbers (adapted from Kohl
and N ielsen, 1997)
It is normally considered good practice to design for a gas flow rate that gives
a pressure drop of less than 3 cm water per meter of packing. In the case in which
the liquid tends to foam, less than 2 cm waterlm is recommended (Kohl and Nielsen,
1997). In bioscrubbing the gas loading rate ranges between 4000 and 10000 m 3/m 2 .h
for volatile compounds readily soluble in water (Kok, 1991; VDI/DIN, 1996), which
corresponds with gas veloeities in the column of 1-3 mls (Fiseher, 1990). The height
of the absorbers used in bioscrubbing range from 2 to 8 m, with 3 m as a good
average (VDI/DIN, 1996). As a consequence the gas retention time in the absorber is
a few seconds.
The water flow in the absorption tower should wet the packing surface as
much as possible. This implies a good distribution over the packing and a sufficiently
large flow rate. The number of liquid streams provided by the feed distributor should
be 10-20 per m2 and liquid redistributors are required every 5-10 tower diameters for
rings, and at least every 7 m for all types of dumped packing. The latter may be good
reason to limit the height of bioscrubber absorbers to 7 m. For a good wetting of the
surface packing about 10 m3 water/m 2 column horizontal section/h is required.
However, to prevent attachment of biomass on the packing, and eventually tower
clogging, the shear ofthe water flow should be sufficiently high. This can be reached
by applying a surface loading rate of at least 20 m3 waterlm 2.h (Kok, 1991; Schippert,
1994). VDI/DIN (1996) recommends a trickling density of 20 to 60 m 3/m 2.h and a
ratio ofliquid/air flow of 0.002-0.003.
The materials used for construction of the absorption tower cylinder should be
resistant to corrosion caused by liquids and gases and thermal!y and mechanical
resistant for the temperatures and loading rates applied. The material of out-door
absorbers should also be UV resistant. Plastics such as polyvinyl chloride,
Bioscrubbers 137
For the design of the absorber column (height, diameter) and water flow rate for a
given gas flow, it is important to know the Henry's law's coefficient in order to
calculate how much water at least is required for a certain elimination efficiency.
Subsequently, mass transfer rate considerations give the required surface area for
interphase mass transfer. From the required surface area, the packing volume can be
calculated for each type of packing material.
When polluted gas is contacted in a counter-current absorption column, the
water leaving the column is brought into contact with the influent gas. The
concentration of a compound in this so called 'rich' water can not be higher than the
concentration in equilibrium with the concentration in the gas phase, according to
Henry's law:
(5.1)
in which
H = dimensionless Henry's law coefficient (g.m- 3 gasi g.m-3 water),
Cg = concentration of a compound in the gas phase (g/m 3 ),
CI = concentration of a compound in the liquid phase (g/m 3).
This implies that the ratio between the water flow and gas flow should be at
least H, otherwise high elimination efficiencies (> 95%) cannot be attained. For this
purpose, the absorption factor is created (Overcamp, 1993):
(5.2)
in which
A = absorption factor (dimensionless),
FI = liquid flow rate (m 3 /h),
Fg = gas flow rate (m 3 /h).
If the concentration in the gas phase is higher than the concentration in the
water phase multiplied by H, in any part of the column, a driving force exists for
transfer ofthe compound from the gas phase to the liquid phase.
The mass transfer in the absorber can be described by the two film theory
developed by Lewis and Whitman (1924). In this model two bulk phases (gas and
liquid) have different concentrations and are not in equilibrium according to Henry's
law. Only at the interphase such equilibrium exists. In a very small film of liquid near
the interface, a concentration profile exists connecting liquid bulk concentration and
interphase concentration. The same is true for the gas phase. In these films the target
molecules move with a certain velocity, depending on the properties of the
compound and the solvent. These velocities are defined in mass transfer rate
coefficients (m/s): both films have different mass transfer rate coefficients, which can
be combined to one overall mass transfer coefficient:
(5.3)
in which
KI = overall mass transfer coefficient (m/s),
kl = partial mass transfer rate coefficient in the liquid phase (m/s),
kg = partial mass transfer rate coefficient in the gas phase (m/s),
mi = distribution coefficient (gas/liquid) of the target compound (-),
(5.4)
The mass transfer from the gas phase to the water phase occurs at a rate F:
(5.5)
where 'a' is the specific interface area (m 2/m 3 ) and F is expressed in (kg/m3 .s).
is the height over which the gas phase concentration target compound is reduced with
a factor 'e', which has a value ofabout 2.7. In bioscrubbers HTU ranges between 0.2
and 2 m (Fischer, 1990). NTU is the number of sequential HTUs required to attain
the desired elimination efficiency. One HTU gives an efficiency of 57%, while 95%
requires three and 99% five HTUs.
1
NTU=ln-- (5.6)
E
1--
100
and
in which E is the elimination efficiency in percentage, and h is the height (m) of the
packing in the absorber.
Equation 5.6 is only true if the absorption water fed to the top of the column
is absolutely free of the compound to be absorbed, which is seldom found in
bioscrubbing. To account for the presence of the target compound in the lean water,
the following formula should be used:
(5.8)
in which
GM = superficial molar mass velocity of gas stream (moles/m2 .h),
LM = superficial molar mass velocity ofliquid stream (moles/m2.h),
X2 = mole fraction solute in liquid fed to top ofthe column,
Yl = mole fraction solute in gas fed to bottom ofthe column,
Y2 = mole fraction solute in gas leaving top ofthe column,
H = dimensionless Henry's law's coefficient (g m- 3 gas / g m-3 water).
Note that the group HGM/L M appears several times in Equation 5.8: it is the
stripping factor, the reciprocal absorption factor (Equation 5.2). Equation 5.8 is only
true if Henry's coefficient is constant over the whole concentration range involved
and requires that temperature does not change in the column (as it changes H).
HTU=~ (5.9)
KgaP
in which P is the total gas pressure ofthe system (atm).
140 J. W van Groenestijn
The most difficult point in practice is the value of Kg or of Kga. The valuc
depends on the nature of the compound, the properties of the gas and the liquid
(viscosity, composition, mixing, turbulence) and temperature. In addition, mixtures
of pollutants in gas make the design even more complex. Therefore pilot plant tests
cannot be avoided. They should give the basis for further scale up calculations using
the formulas described above. The given formulas can also be used to compare
absorbers, to estimate if existing absorbers can be approved and how they react on
changes in, among others, gas flow rate, liquid flow rate, gas concentrations, liquid
concentrations, height ofthe packing.
Formulas 5.1 to 5.9 were obtained from various literature sources (Ottengraf,
1986; Fischer, 1990; Riet and Tramper, 1991; Overcamp, 1993; Schippert, 1994;
VDIIDIN, 1996; Kohl and Nielsen, 1997) and adapted for this chapter.
3. Bioreactors
The aqueous effluent from absorbers is loadcd with absorbed pollutants and can be
regenerated in a bioreactor. In this regeneration process the pollutants are
biodegraded and converted into CO 2 , H20 and mineral products. As a resul! the water
can be reused in the absorber. Most bioreactors in bioscrubbers arc tanks with a
suspension of activated sludge and spargers for bubble aeration. The properties and
design of such bioreactors show great similarity with activated sludge tanks for
wastewater treatment. The most important difference is that the hydraulic retention
time is much longer, generally the same as the sludge retention time. The
consequence is that generally no measures are required for sludge retention, such as
sedimentation and sludge retum and addition of support material for biomass
attachment. Because of the low hydraulic loading rate, the concentration of the
activated sludge can be higher than that in activated sludge tanks in wastewater
treatment systems. Nevertheless, enhanced sludge retention in bioscrubber
bioreactors can be an option in case micro-organisms have to be retained with
extreme low growth rates (e.g. nitrifiers at low temperatures) or in case the water has
to be refreshed at a high rate because of accumulation of degradation products.
• Decide which concentration of the target compound in the lean solvent is desired
(connection to the design ofthe absorber);
• Estimate the growth rate ofthe micro-organisms involved;
• Estimate the specific substrate conversion rate;
• Calculate the required amount of biomass in the reactor;
• Calculate the required addition of nutrients;
• Calculate the required addition oftitrants;
• Calculate the rate of accumulation of reaction products, nutrients and titrants;
• Calculate the dilution rate ofthe reactor (water refreshment);
• Calculate the amount of oxygen required and design the aeration system;
• Calculate the volume ofthe bioreactoL
Bioscrubbers 141
Knowledge on the growth rate is required for the ca1culation of the minimum
sludge retention time and may also be used in ca1culation of the specific substrate
conversion rate. The growth rate is dependent on environmental factors such as
temperature, pH, ionic strength, presence of toxic compounds and the substrate
concentration. The dependence on the substrate concentration is expressed by the
Monod equation as also explained in previous chapters:
(5.10)
in which
).l = specific growth rate (g biomass/g biomass .h),
Ilmax = maximum specific growth rate (g biomass/g biomass .h),
CI = substrate concentration (g/m3),
Ks = Monod constant or substrate affinity constant (g/m3).
The total rate of consumption, expressed per gram ofbiomass dry weight, is:
1!..+m (5.11)
y
142 J W. van Groenestijn
2. Use ofthe Michaelis-Menten equation, originally developed for enzymes, but also
true for whole cells:
v (5.12)
in which
V = specific substrate conversion rate (g substrate/g dry biomass .h),
V max = maximum specific substrate conversion rate (g substrate/g dry biomass .h),
Km = Michaelis-Menten constant (g/m\
Using the substrate conversion rate and the expected loading rate of the
pollutant(s), the required amount of biomass can be calculated. Note that the water
from the absorber sometimes can contain COD concentrations as high as 5000 mgl!.
In bioscrubber bioreactor design the kinetic parameters as used in Equations
5.10 and 5.11 are not always known and if the waste gas contains mixtures of
biodegradable compounds, calculation becomes too complex. Therefore design rules
of thumb are used, while the equations above can be used to estimate the effect of
changes in operation and design. Mostly the bioreactor is oversized to guarantee
stability and to cope with fluctuating loading rates. According to the VDI/DIN
guidelines (1996), the design should be based on the maximum half hours average of
the absorbed load. The concentration of biomass in bioscrubber bioreactors ranges
between 1 and 15 g dry weight (Schippert, 1994). Sludge concentrations higher than
15 g/Ilead to too much clogging ofthe absorber packing (VDIIDIN, 1996). Ottengraf
(1986) recommends evcn lower sludge conccntrations: not more than 5-8 g dry
weightl!. The volumetric conversion rate of bioscrubber bioreactors is 20-200 g/m 3.h
(Schippert, 1994) and maximum 400 g/m 3 .h for readily biodegradable compounds
(Fischer, 1990; VDI/DIN, 1996), while the sludge loading rate is 0.005-0.006 g
substrate/g biomass dry weight . h. The yield factor observed in practice ranges
between 0.1 and 0.4 g dry sludge/g substrate. The bioreactor can be started up by
inoculation with activated sludge from waste water treatment plants.
Because of the completely mixed character of the liquid in the bioreactor, the
concentrations ofthe biodegradable compounds are low in the entire system, which is
an advantage in case these compounds are toxic (e.g., aromatic compounds and
formaldehyde). In biofilters, however, high (toxic) concentrations may exist at the
biofilm surface.
The growth of biomass requires nutrients. The amount can be estimated from
the sludge production rate (10) and element composition of biomass. According to
Stanier et al. (1978) the average microbial cell contains (based on dry biomass) 50%
C, 20% 0,14% N, 8% H, 3% P, 1% S, 1% K, 1% Na, 0.5% Ca, 0.5% Mg, 0.5% CI,
0.2% Fe, othcr elements 0.3%. Tracc clemcnts generally are present in the waste gas,
the used water and in the other raw materials, a part of the macro elements may also
be present in the gas (N and S compounds, dust) or in the used tap water (Ca and
Mg). Often, P is thc limiting factor and N and Parc added as the only nutrients, but
care should be taken not to create element limitation for growth.
Bioscrubbers 143
flow rate (m3/h) aud bioreactor volume (m3) ranges between 100 and 3000, with
1000 as a balauced average. Compared with biofilters, which are mostly loaded with
100 m3 gas/m3 filter bed .h, the volume of bioscrubbers is almost an order of
magnitude lower thau the volume ofbiofilters.
The pump between the bioreactor and the absorber should be a positive
displacement pump or a slow running centrifugal pump, to minimise destruction of
sludge flocs. The pumps should be cOITosion resistant aud their shaft seal should be
able to withstaud solids. A dry running protection is recommended.
In the early nineteen eighties bioscrubbers were installed to treat gases from
enamelling ovens (alcohols, glycols, ketones, glycolether, aromatic compounds aud
resins), incinerators, foundries (amines, phenol, formaldehyde aud ammonia) aud fat
smelteries (Ottengraf, 1987).
One of the ear1y comprehensive reports on a successfu1 bioscrubber
application was that from Schippert (1986), who described how waste gases from a
paint booth in Ma1mo were treated. The factory emitted 35000 to 60000 Bm3/h with
30-45 kg VOC aud 2 kg resin aerosol per hour at a temperature of 160 aC. The gas
first pas sed aventuri scrubber for cooling and remova1 ofthe aerosol. In this scrubber
1500 kg water evaporated aud the heat (200 kW) was recovered. Subsequently two
scrubbers with a diameter of 4 m aud a height of 6 m were used aud two activated
sludge tanks with a total added volume of 280 m3 for the regeneration of the
absorption 1iquid. Sludge retum was mauaged via flotation aud waste water was
produced at a rate of 0.5 m3/h. Nutrients were added to maintain a high microbial
activity: 0.15 kg Na2HP04, 0.6 kg (NH4)2S04 aud 0.1 autifoam agent per hour. 180
kW energy was required at full capacity aud minor amounts of NaOH as a titraut.
99% remova1 ofVOCs was observed from a mixture ofbuty1 glycol, n-butanol, ethyl
glycol, isobutanol, xylene aud MIBK (methyl isobutyl ketone) in air. Xylene aud
MIBK showed the poorest elimination efficiencies (70%) but their concentration in
the influent gas was only 10w.
After three years the author reported again about this bioscrubber. The
e1imination efficiency still was more than 99%, of which 99% was attained in the
first stage. Therefore, it was conc1uded that the bioscrubber was over-dimensioned.
Another problem was the attachment of biomass on the scrubber packing. It was
observed that this effect coincided with the addition of excess amounts of nitrogen in
the second stage. The mechanism behind this effect was not studied further
(Schippert, 1989a).
Another early report of a bioscrubber treating gases from a paint booth was
from Beyreitz (1989). A biofilter aud a bioscrubber were 10aded simultaueously with
a gas containing acetone, methy1 ethyl ketone, toluene, butyl acetate, 2-propauol aud
di-acetone alcoho1, to compare their performance. The biofilter had a loading rate of
70 m 3 /m 2/h, the bioscrubber had a higher surface loading rate because of its smaller
size. The biofilter removed 90% ofthe VOCs present, ofwhich toluene was the most
problematic with only 51 % elimination. The bioscrubber removed 80% VOCs of
Bioscrubbers 145
which 0% toluene. The conclusion was that bioscrubbers are attractive for removal of
hydrophilic compounds, because of its reduced size, but biofilters still are needed for
removal of hydrophobic compounds. The author suggested that a combination of a
bioscrubber and a biofilter might save space, which could be an important
consideration in an industrial environment.
An example of a bioscrubber at a foundry can be found in a paper written by
Buren (1989). The bioscrubber treated 36000 Bm3/h waste gas containing phenol,
formaldehyde and ammonia. The bioscrubber comprised an absorber column,
followed by a clarifier (a plate settler for removal of dust) and a bioreactor. The
bioreactor was a hydrolift reactor in which air and water were introduced at the
bottom section and activated carbon particIes with aUached biofilm were fluidised.
The advantage of the use of activated carbon as a support material was the buffering
of concentration fluctuations. The bioscrubber reduced the phenol concentration from
50 to less than 3 ppmv, the formaldehyde concentration from 5 to less than 0.5 ppmv,
while ammonia (30 ppmv) was removed with an efficiency of at least 50%.
More bioscrubbers for the removal of phenol and formaldehyde are described
by Huckschlag (1992). Pilot plant investigations have been carried out at the sites of
wood factories, textile plants and glass wool manufacturers between 1985 and 1991.
Phenol always could be removed at least 97% and formaldehyde at least 85%.
Interesting details on the design and operation of a state of the art bioscrubber can be
found in Kellner and Flauger (1998). The bioscrubber cleans waste gases from a
coating process that contains a mixture of hydrophilic VOCs of which 84% is
acetone. The air flow rate is 20000 m3/h, the acetone concentration 800-2000 mg/m3
and the temperature 22°C. The bioscrubber comprises a packed bed co-current
scrubber and an activated sludge tank. The scrubber has a column diameter of 2 m
and a packing height of 2 m, while the volume of the activated sludge tank is 140 m 3 .
The activated sludge system also comprises a sludge sedimentation tank and sludge
recycling. Fertilizers are added to support the growth of micro-organisms: 24 kg/day
during starting up and 50 kg/week during steady state operation. The biomass
concentration in the activated sludge tank is 2-3 g dry weightll and 5 m3 of the
recirculation liquid is discharged in the sewer each day.
At the start of the operation in 1995 a liquid loading rate of 10 m3/m2 .h was
used. This appeared to be too low: the packing was clogged with biomass and the gas
pressure drop increased up to 1800 Pa. Pilot plant studies carried out by Loy et al.
(1998) revealed that a lower packing height and a higher liquid loading rate (28
m3/m2.h) prevented clogging of the absorber packing. These insights were
implemented on full scale: the packing height was reduced from 2 m to 1.5 m and the
liquid loading rate was increased to 24 m3/m2 .h. From that moment a high cleaning
efficiency could be obtained without any problems of clogging.
Bioscrubbers are very suitable for treating gases in which organic nitrogen
compounds are present. The production of ammonia as a result of biodegradation and
subsequent nitrate accumulation by nitrification may yield problems in biofilters. In
bioscrubbers, however, control of the pH and concentration of inorganics is very
easy. A good example is the bioscrubber described by Hansen and Rindel (1992) for
the treatment ofwaste gases from a fish feed production factory. 25000 m3 gas/h was
146 J W van Groenestijn
A prerequisite is that the compounds to be treated in the waste gas are the
same as or show sufficient similarity with compounds introduced in the waste water
treatment plant.
Bioscrubbers 147
Table 5.2. Applications of bioscrubbers at various industries (adapted from VDI/D1N, 1996)
Conventional bioscrubbers can only be used for compounds which are readily soluble
in water. Thc !imit is set by a Henry's law's coefficient of 0.01. The addition of an
organic solvent to the water phase, however, can make bioscrubbers fit for
Bioscrubbers 149
phenol, naphthalene and pentachlorophenol have been tested and solvents as pristane,
dibutyl phtalate, hexadecane, dodecane, heptamethyl nonane, silicon oiI and paraffin
oiI were used. Not all solvents meet the demands given above. In continuous
degradation experiments with long durations, ali kinds of negative effects can appear.
Gardin et al. (1999) further selected suitable solvents. Based on known physical
properties pristane, isopar V, isopar L, perfluoro hydrocarbons and silicon oiI were
preselected. However, biological experiments revealed that pristane, isopar V and L
were not inert: they were degraded by microorganisms, while perfluoro hydrocarbons
were toxic. Silicon oii seems the best choice up to now. It was proven that the
presence of silicon oii in a aqueous medium could greatly enhance the growth of
micro-organisms on xylene as a substrate. Besides the improvement of
bioavailability, solvents can reduce the toxicity of compounds (by decreasing the
concentration in the water phase) and can act as a buffer system for fluctuating loads
of hydrophobic or toxic substrates (Deziel et al., 1999; Gardin et al., 1999).
According to Deziel et al. (1999) it is important to create an aqueous/solvent
interphase area as large as possible. An optimal phase ratio exists that will generate
the highest interphase area. This ratio depends on the physical conformation of the
bioreactor, properties of the solvent and the mixing rate. 2~O% solvent in water
gives the highest areas. A higher oii phase ratio may lead to larger drop sizes (Deziel
et al., 1999) or even phase inversion (Groenestijn and Lake, 1999). A small drop size
may be created by emulsifiers, inc1uding the natural emulsifiers excreted by the
microorganisms in the system.
As with aqueous bioscrubbers, water and sludge in two-liquid-phase
bioscrubbers have to be discharged after some time of operation. In running full-scale
systems this is achieved by separation ofthe two phases ofthe waste liquid stream by
centrifugation, followed by recyc1ing of the expensive organic phase and discharge of
the aqueous sludge suspension. Not more than 3% of the organic solvent is lost
annually (Keramchemie, personal communication), which in addition limits
environmental damage.
Separation of the aqueous and organic phase plays an important role in the
bioscrubber deve10ped by Cesario and co-workers (1992). They propose a
combination of a spray tower and a liquid-impelled loop reactor. In this system a
water-immiscible organic liquid with a high solvent capacity for the pollutant is
recyc1ed between the absorber and the bioreactor. The latter is designed as a liquid-
impelled loop reactor, a liquid/liquid contactor which contains the culture medium
and the cells (Tramper et al., 1987). This reactor comprises a riser and a down-
comer. The organic solvent is introduced at the bottom ofthe riser and causes the low
density water/solvent mixture to rise. At the top of the reactor the two phases are
separated. The organic phase is recirculated via the spray scrubber to the bottom of
the riser, while the aqueous phase is recirculated via the downcomer. Without
bacteria the system works perfectly, however, phase separation becomes difficult
when free suspended bacteria are present (Cesărio and Tramper, personal
communication).
anaerobic conditions. Parker et al. (1998) used scrubbers and anaerobic reactors of
the UASB type to degrade perchloroethylene. As chlorinated hydrocarbons are
relatively insoluble in water, an organic solvent was added to the scrubbing liquid.
One of the organic solvents tested was vegetable oiI. In addition, anaerobic
bioscrubbers are used for elimination ofNOx and SOx (see NOx and SOx sections).
5.5 FOAMS
Bioscrubbers as developed by Hansen (1998) can remove more than 99% of H2S
from aerobic gases. In the bioreactors the sulphide is converted to sulphate, a reaction
that needs alkali addition for pH control and frequent water refreshment to control
salt concentration. Alternatively, the absorbed sulphide can be biologically converted
to eIemental sulphur. This incomplete oxidation can be carried out by bacteria from
the genus Thiobaci/lus if subjected to oxygen limited, but aerated, conditions. Such
system is described by Janssen et al. (1997). A pilot scale bioscrubber was used for
treatment of 160 m 3 sour gas per hour from a refinery. The influent concentration
contained 70-500 ppmv H2S and the effluent concentration O ppmv. This way less
152 J W van Groenestijn
caustic soda is required for pH control as the alkalinity can be recycled over the
bioreactor and the absorber.
Natural gas, biogas, synthesis gas and Claus tail gas mostly contain HzS. In large
scale (> 15 tons S/day) gas treatment, amine absorbers and Claus plants can be used
to remove HzS. For smaUer quantities, liquid redox systems, based on reaction with
iron chelates, are used. Bioscrubbers may be an alternative for these redox systems. A
system similar to HzS removal from aerobic gases can be applied to clean anaerobic
gases. According to Janssen et al. (l999a; 2000) the technology is competitive in the
0.1-15 tons S/day range. The reactions in the absorber and the bioreactor are
respectively:
2 Fe z+ + HzO + 1/2 Oz ~ 2 Fe 3+ + 2 OR
Pagella and co-workers revealed that a pH as low as 1.5 was acceptable for
this reaction. A pH of I appeared lethal. The system was further worked out by
Pagella and De Faveri (2000) in a laboratory scale test using a bubble column
absorber with a: gas residence time of 1.5-2.3 s and a tixed bed bioreactor. The
optimum pH for growth of the bacteria used to oxidise the ferrous ions appeared to
be 2.2.
SOx can be removed from flue gases by scrubbing with dilute solutions of caustic
soda or limestone. However, in these processes the costs for chemi caIs are
experienced as high and products as disodium sulphate can hardly be disposed
(Cetinkaya el al., 2000). A biological alternative was developed (Buisman el al.,
1994; Cetinkaya el al., 2000; Janssen el al., 2000). In this bioscrubber the hot gases
pass an absorber in form of a reverse jet wet scrubber in which particulates and SOx
are absorbed. The most important reactions are:
The latter reaction concerns only a part of the NaHS0 3 formed in the tirst
reaction. The liquid from the absorber is transferred to an anaerobic reactor in which
154 J W van Groenestijn
the sulphites and sulphates are biologically converted to sulphide. For this process an
electron donor is required. For large scale applications H2 gas is preferred, while in
small-scale plants also methanol and ethanol may be used (H2 generation on small
scale is relatively costly). The reactions involved are:
Makeup
NaOH Anaerobic Aerobic
reactor reactor
Figure 5.2. Flow sheet of a bioscrubber for SOx removal from flue gases (adapted from
Cetinkaya el al., 2000).
Pilot plant experiments have been carried out at a 600 MW power plant that
produced 2 mi/lion m 3 flue gas per hour. 6000 m3/h gas with a temperature of 120 °C
was used for the experiments. The plant comprised a 6 m high absorber tower and a
10 m high anaerobic 'Internal Circulation' reactor, in which gas circulated by an
external compressor for a good mixing. The aerobic reactor was an airlift loop
reactor. The water recycle flow was varied from O to 6 m 3/h and the water bleed from
O to 500 IIh. The water from the absorber had a pH of 7-8. Not higher, because that
led to pH problems in the aerobic bioreactor in which an alkaline reaction took place.
The first experiments were carried out using a thermophilic anaerobic reactor (50 0c)
and ethanol as electron donor. The start-up took six weeks. The second reactor
started with the production mainly of sulphate, but after increasing sulphide loading
Bioscrubbers 155
rates, mainly sulphur was produced. The plant was loaded with 6 kg S02Jh and the
SOx removal efficiency was 98% (Buisman et al., 1994; Janssen et al., 2000).
7. NO x removal
A bioscrubber for the removal ofNO x from flue gases is described by Cetinkaya and
co-workers (2000). The problem connected to NO x removal from flue gases is that
95% of the NO x is NO, a compound poor1y soluble in water. To overcome this
solubility problem Fe(II)EDTA is used in the scrubber liquid to react with NO. As a
result, Fe(II)[EDTA]N0 2-, a nitrosyl complex, is forrned and NO is absorbed from
the gas at a high rate, at any temperature. The scrubber liquid containing the absorbed
N0 2 and the nitrosyl complex is subsequently transferred to an anoxic bioreactor in
which biological denitrification takes place. The nitrogen compounds mentioned are
reduced to dinitrogen gas using an electron donor, e.g., ethanol. The Fe(II)EDT A in
the liquid can be reused again in the absorber. Removal efficiencies of more than
80% can be achieved.
8. NH3 removal
In the latter reaction (H) represents an electron donor (reductor). This can be
an organic compound, sulphide or H2. Note that the overall reaction is not acidic nor
alkaline. Therefore, a denitrification step in the bioscrubber is attractive because of
the better pH control and because the water can be used a longer time, since this way
no inorganic compounds are accumulated.
Nitrifying micro-organisms have low growth rates. The generation times
range from 3 to 10 days depending on environmental conditions. Since the sludge age
of bioscrubber bioreactors can be very high, nitrification is possible. Ammonia
removal by bioscrubbers has been reported manifold. An example can be found in
Hansen and Rindel (1992): a bioscrubber for the treatment of gases from a fish feed
factory. Nitrate accumulated in the bioreactor liquid, because no denitrification step
was incorporated.
Hvidtfeldt Rasmussen et al. (1994) developed a bioscrubber in which both
nitrification and denitrification took place. The bioscrubber was installed to treat
40000 m3Jh waste gas from a fish feed factory. During production hours organic
compounds were absorbed in the absorber at which also some nitrification took
place, while denitrification took place in the anoxic sump under the column. In the
production intermission periods, further nitrification took place in the same sump,
156 J W van Groeneslijn
but undemeath aerobic conditions. As organic compounds absorbed from the gas
served as electron donor for the denitrification process, addition of chemicals, such
as methanol, were not required.
Groenestijn el al. (1997) propose the use of separate absorbers, nitrification
reactors and denitrification reactors for the removal of ammonia from waste gases
from intensive livestock breeding. Many decentral absorbers can be connected to one
central biological treatment unit. This way ammonia is transported through small
water pipes rather than large gas pipes. Nitrification reactors could be constructed as
trickling filters with natural air draft. The denitrification process can be carried out
with methanol as electron donor. Based on laboratory experiments a 2 m3 absorber, a
4 m3 trickling filter, and a 1 m3 denitrification reactor should be used to treat 8000 m3
waste gasJh containing 15 mg NH 3/m3 .
9. Costs
First statements about costs in review papers are discussed and subsequently these
are checked with data from individual reports. For ca1culation of amounts in Euros
(€), the exchange rates of September 2000 are used.
According to Kok (1991) the investment costs of bioscrubbers range from
NLG 20 (€ 9) to NLG 60 (€ 27) per m3Jh gas flow rate. The bioreactor accounts for
the largest part of these costs. According to Menig el al. (1997) a bioscrubber for
10000 m3Jh costs DM 500000 (€ 256000) and one for 60000 m3Jh DM 1200000 (€
613000), which means DM 20-50 (E 10-51) per m3Jh, depending on the size of the
bioscrubber.
In one of the earliest Dutch review papers on bioscrubbing (Joziasse and
Wiering, 1992) operation costs inc1uding capital depreciation range from NLG 1.20
to 4.50 (€ 0.54-2.04) per 1000 m3 treated gas in the 30000-130000 m 3Jh flow rate
range. Kok (1991) gives a wider range: NLG 1-5 (E 0.45-2.27) /1000 m3 . According
to Menig el al. (1997) the exact operation costs, inc1uding the capital costs, depend
on the time the bioscrubber is operational (day/night, weekends, etc.). In a certain
bioscrubber that operated 8000 h per year treatment of each 1000 m3 gas cost DM 1.3
(E 0.66), while DM 2.3 (€ 1.18) costs would be made ifthe same bioscrubber would
operate for only 3000 hours per year. According to the authors catalytic oxidation is
50% more expensive and adsorption even 100%. According to Kok (1991) 60% of
the operating costs of bioscrubbers are capital costs. Energy can be the next
important cost factor. Bioscrubbers that treat gases containing less than 0.5 g
VOC/m3 consume 1.5-3 kWhl1000 m3 treated gas. If the VOC concentration is
higher, the energy consumption increases.
The operation costs also can be expressed per kg VOC removed. Kok (1992)
ranges the costs for bioscrubbing between NLG 2 (€ 0.91) and NLG 5 (€ 2.27) per kg
VOC removed, with the lowest values for off-gases with high concentrations and
compounds readily soluble in water.
Specific cost analyses can be found in Kellner and Flauger (1998) in which a
bioscrubber for treatment of 20000 m3/h costs DM 450000 (€ 230000). According to
the authors this is less than many other bioscrubbers which would have cost DM
Bioscrubbers 157
700000 (€ 358000). Neverthe1ess, their investment costs are 40% higher than that for
a biofilter, but 35% lower than required for adsorption. The costs given are low, but
within the ranges given above. The bioscrubber described by Biiren (1989) had
operation costs exc1uding capital costs of DM 0.5 (E 0.26) per 1000 m3 gas. A
bioscrubber for treatment of 120000 m3 gas/h described by Fischer (1990) costs DM
1100000 (E 562000), which can be regarded as lower than the ranges given above.
The operation costs exc1uding capital costs were DM 0.33-0.45 (E 0.17-0.23) per
1000 m3 gas, of which 80-90% were electricity costs. Standefer and Willingham
(1998) compared their combination of a bioscrubber and a biofilter with sole
biofilters. In their specific case, the investment costs connected to the combination
were 20% lower than those of a biofilter, and the operation costs were 40% lower
(US$ 0.09 or € 0.10411000 m3 exc1uding capital costs). Incineration would have cost
nine times more.
Although Frohlich (1994) did not give exact cost figures for the 41000 m 3/h
capacity bioscrubber described, the electricity use was 60-90 kW and the water use
100-500 l/h, while the chemi cal costs were 17 times smaller than the e1ectricity
costs. According to Hansen (1998) bioscrubbing of gases containing 10 mg H 2S/m3 is
2 times more cost-effective compared with chemical scrubbing. This factor grows to
3 ifthe H2 S concentration is 50 mg/m 3 .
Janssen et al. (1997) arrived at operation costs for H2S removal from aerobic
gases, comparable with those described above. US$ 400000 (€ 464000) inc1uding
capital costs is required annually for treatment of 50000 m3 gas/h. In case the
operation was continuous, this would mean US$ 0.91 or € 1.0611 000 m 3 .
In summary it can be stated that the investment costs for bioscrubbers range
from € 10 to € 25 per m3 gas/h, mainly depending on the size. These costs may be
about 40% higher than those of biofilters. The operation costs range from € 1 to € 3
per 1000 m3 gas treated, mainly depending on the concentration, the solubility of the
compounds in water and the number of operating hours per year. High
concentrations, high solubility and a high number of operation hours lead to lower
operation costs. These costs can be higher or lower than those of biofilters. For gases
containing VOCs with Henry's law's coefficients lower than 0.001 and in
concentrations higher than 0.5-1 g VOC/m 3 bioscrubbers may be more cost-
effective.
According to Cetinkaya et al. (2000) bioscrubbing ofNO x from flue gases costs US$
0.81 or € 0.94/lb N and bioscrubbing of SOx costs US$ 333 (€ 386) per ton S, which
is 2.5 lower than SOx using caustic soda scrubbers. The operational costs of the
biological process for SOx removal are lower than those of the caustic soda process,
while the investment costs are higher. The pay back of the higher capital investment
will be site specific and based on the sulphur loading and flue gas flow rate.
Paybacks within two years can easily be achieved at higher sulphur loads. According
to Grootaerd et al. (1997) the operational costs for biological SOx are slightly lower
than that of the limestone forced oxidation process. Only if the gypsum market
becomes saturated the biological process becomes competitive. In addition, the
growing concern about heavy metals in gypsum from the limestone process may
influence decisions on flue gas treatment.
158 J W van Groenestijn
A bioscrubber for the removal of 5000 ppmv H2S from 42000 Nm3 natural
gas per hour costs US$ 5500000 (€ 6380000) (Janssen et al., 1999a). The operation
costs excluding depreciation of the capital costs amount US$ 430000 (€ 500000)
annually (about US$ 1.17 or € 1.36 per 1000 m\ which is lower than the operation
costs ofliquid redox technology.
Comparable with biofilters and biotrickling filters, bioscrubbers can be cost effective
for treating waste gases containing VOC concentrations lower than a few g/m3. The
application of bioscrubbers can be more attractive than the use of biofilters if the gas
contains relatively high concentrations ( > 0.5 g/m 3) of hydrophilic compounds such
as alcohols, aldehydes, fatty acids and glycols. In addition, bioscrubbers can be cost-
effective for the treatment of gases containing N, S and halogenated compounds, and
attractive in case land area is limited. Combinations of bioscrubbers and polishing
steps can be interesting for treatment of gases with mixtures of hydrophobic and
hydrophilic compounds.
Considerable progress is made in the development of bioscrubbers for the
treatment of flue gases and anaerobic gases. The development of a bioscrubber for
NOx is still in its infancy, but promising. More attention still should be given to the
development of bioscrubbers containing alternative solvents. The addition of organic
absorbents, solid absorbents, adsorbents and reagents to the aqueous phase can
facilitate the absorption ofhydrophobic compounds such as alkanes and NO.
At present, biological waste gas treatment accounts for only about 2% of the
total world waste gas treatment financial turn over. By developments as described
above, physico-chemical processes can be substituted by biological ones and this
substitution process may be the most important opportunity for growth of the turn
over in biological waste gas treatment.
Abbreviations
Acknowledgement
The author gratefully acknowledges the support given by TNO Environment, Energy and Process
Innovation, Apeldoorn, the Netherlands, to write this chapter.
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1996. VOI Verlag (Publisher), Dtisseldorf, Germany.
CHAPTER 6 MEMBRANE BIOREACTORS
Sarina J. ERGAS
1. Introduction
163
C. Keflfles afld M. C. Veiga (eds.), Bioreactorsfor Waste Gas Treatmeflt, 163-177.
© 2001 Kluwer Academic Publishers.
164 S. J Ergas
Disadvantages of HFMBs for waste gas treatment include high capital costs
and that the technology has not been demonstrated at full-scale .
Hollow fibre membrane bioreactors have been used in a number of pollution control
applications inc1uding:
•
Contaminated
InJet Air
MOOngI
Recirculation
Flow
HolJow
Fiber
Membranes
Figure 6.1. Schematic of a hollow fibre membrane bioreactor for biological air polllltion
control (after Shllmway, 1997).
Membrane bioreactors 165
Membrane bioreactors are most often used for separation of biomass. The
ultrafiltration of microfiltration membranes are used as a substitute for
sedimentat ion. These systems are used to produce high quality effluent and/or
provide high solids retention times without washout of biomass. These applications
are well documented in the literature and are outside the scope of this discussion
(Stephenson el al., 2000).
Gas to liquid transfer membrane systems were first introduced for use in
blood oxygenation and have been studied extensively for this application (Lund el
al., 1996). Pollution control research into membrane aeration HFMBs has been
focused on the enhancement of oxygen transfer in high oxygen demanding
applications such as the treatment of high strength industrial waste waters
(Yamagiwa el al., 1998) and nitrification (Brindle and Stephenson, 1996b; Brindle el
al., 1998). These systems have also been used for bioreactors degrading VOCs, since
the membranes allow for reactor aeration without stripping volatile compounds to the
atmosphere (Pressman el al., 1999). Owing to the low solubility of oxygen, oxygen
transfer often limits aerobic degradation of high oxygen demanding waste waters.
Many facilities switch from atmospheric air to pure oxygen to enhance oxygen mass
transfer; however, conventional oxygenation systems have high power requirements
and are incompatible with attached growth reactors (Stephenson el al., 2000).
Hollow fibre membranes provide a very high surface area for transfer of oxygen
directly to the biofilm. Hydrophobic hollow fibres have been developed with sealed
hydrophilic ends that enable 100% utilisation efficiency in gas to liquid mass transfer
applications (Ahmed and Semmens, 1992a, I 992b).
A novel application of HFMB gas transfer technology, hydrogenotrophic
denitrification of drinking water, has been investigated by several researchers
(GantzerI995; Lee and Rittmann, 2000; Ergas and Reuss; 2001). A number of
common genera of bacteria can use hydrogen as an electron donor and nitrate as an
electron acceptor under anoxic conditions. These organisms have been shown to
denitrify nitrate contaminated drinking water to acceptable levels. Disadvantages of
hydrogenotrophic denitrification include lower denitrification rates and the difficulty
in dissolving sufficient quantities of hydrogen into the water owing to its low
solubility. Use of HFMBs has been shown to support high biomass densities and
improve hydrogen mass transfer rates while preventing the waste of excess hydrogen
and avoiding accumulation of explosive gasses in a confined space.
Extractive membrane bioreactors have been used to biologically trea!
industrial waste waters in the presence of high concentrations of acids, bases and
salts that can inhibit degradation (Livingston, 1994; Livingston el al., 1998).
Extractive membrane bioreactors utilise dense silicone membranes that selectively
extract organic pollutants such as cholorethanes, chlorobenzenes and toluene, from
polar and ionic compounds. A VOC degrading biofilm grows on the surface of the
membranes creating a driving force for mass transfer. Owing to the selectivity of the
membranes, the biofilm is isolated from the harsh conditions in the waste water to
ensure high biodegradation rates.
166 S. J Ergas
3. Membrane fundamentals
A membrane separates two distinct bulk phases of a system while allowing the
transport of compounds from one phase to the other. In waste gas treatment
applications, gases are most often blown through the lumen (inside) of tubes made
from membrane materials. Pollutants from the gas phase diffuse through the
membranes to a liquid phase on the shell si de (outside) of the membranes. The
membranes also serve as a support for the microbi al population. Once in the Iiquid,
compounds are biodegraded, creating a concentration gradient which serves as a
driving force for mass transfer.
Membranes are available in a wide variety of materials, porosities, and pore
sizes. For successful application, membrane materials must strike a balance between
reasonable mechanical strength, high permeability and high selectivity (Stephenson
el al., 2000). For microporous membranes, high selectivity requires a membrane
material with a narrow range of pore sizes and high permeability requires a
membrane material with a high porosity.
Dense and porous membranes are fundamentaIly different from each other.
Dense membranes rely on physical-chemical interactions between the permeating
compounds and the membrane materials. The mass transfer rate through a dense
membrane depends on the solubility and the diffusivity of the permeating compound
in the dense matrix (Reij el al., 1998). Dense membranes are limited to polymeric
materiaIs, such as latex and silicone, they can be operated at high gas pressures, are
resistant to chemical and mechanical abrasion (Fitch el al., 2000; Stephenson el al.,
2000). Dense membranes have also been shown to be more resistant to biofouling
than porous membranes (Cote el al., 1988; 1989), possibly because the hydrophobic
nature of silicone resists attachment of microorganisms.
Microporous hydrophobic membranes are most often used in gas transfer
applications because they provide a high gas permeability, while not aIlowing
transport of water across the membrane. The membrane pores remain gas filled and
compounds transfer from the gas stream through the membrane pores by gaseous
diffusion. At excess liquid side pressures above the critical pressure, M> cr. water
enters the pores of the membranes, dramatically decreasing mass transfer rates
(Ergas and Reuss, 2001). Gas side pressures greater than the bubble point result in
bubble formation in the liquid phase (Semmens et al., 1999). Thus over the excess
pressure range of O to ~Pcr the gas-liquid interface is immobilised at the mouth ofthe
membrane pore on the liquid side (Sikar, 1992).
Microporous hydrophobic membrane materials include polytetrafluorethylene
(PTFE), polypropylene, Teflon™, Gortex™ (PTFE/nylon) and other composites.
Hydrophobic microporous membranes coated with an extremely thin layer of
silicone have aIso been investigated (Sikar, 1992). The thin silicone layer increases
mass transfer resistance but also decrease biofouling. Microporous hydrophobic
membranes are available with pore diameters between 0.1 and 1.0 f.U11 (Stephenson el
al., 2000). The membranes are manufactured as small diameter (200-400 )lm ID)
hoIlow fibre bundles that provide surface area to volume ratios as high as 30 to 100
cm'! (Sirkar, 1992). This is an order of magnitude greater than equivaIent sized
packed towers.
Gas to liquid transfer can also be carried out using microporous hydrophilic
membranes such as polysulfone and cellulose membranes. In these applications, gas
Membrane bioreaclors 167
pressure must be higher than liquid side pressures. The gas-liquid interface is thus
immobilised at the pore mouth on the gas side ofthe membrane.
Control of biomass thickness has been shown to be a key operational
consideration in continuously operated HFMBs for aeration of waste waters
(Stephenson el al., 2000) and biological waste gas treatment (Ergas and McGrath,
1997). Decreased HFMB performance has been observed in bioreactors afier the
development of a thick biofilm owing to substrate mass transfer limitations,
membrane fibre plugging, decreased biomass activity, and/or metabolite
accumulation (Brindle and Stevenson 1996a; Freitas dos Santos el al. 1997). Hollow
fibre bundles also tend to clump together when biofilm growth is high. resulting in
fibre tangling and reduction of available membrane surface area. Several operational
strategies have been used to maintain film thickness at an optimum level including
the use of cross-flow membrane configurations (Ahmed and Semmens, 1996) and
periodic shearing of biomass from the membranes using high liquid velocities
combined with scouring with gas bubbles (Pankhania el al., 1994; Dolasa and Ergas,
2000).
4. Research overview
A summary of the laboratory scale investigations of HFMBs for air pollution control
is shown in Table 6.1. In an early study by Hartmans et al. (1992) a HFMB was used
to control air emissions of toluene and dichloromethane. Mass transfer coefficients
were determined for a number of different membrane materials. Using the
experimentally determined mass transfer coefficients, dichloromethane removal was
simulated. Results of simulations suggested that a significantly lower reactor volume
would be required for a HFMB than for a biotrickling filter. Greater than 95%
removal of toluene and dichloromethane were observed in experiments with aflat
sheet membrane bioreactor.
Parvatiyar el al. (1996a) used a two module-in-series polysulfone HFMB to
investigate toluene removal from a contaminated airstream. Toluene removal reached
84% with a 16 second gas residence time and an inlet concentration of 600 ppmv. A
similar experimental system was used by the authors to study degradation of
trichloroethylene (TCE) (Parvatiyar et al., 1996b). The biofilm was initially
acclimated to toluene, then gradually weaned from a toluenerrCE mixture to 100%
TCE. A 30% TCE removal efficiency was achieved with a 36 second gas residence
time.
Fitch et al. (2000) compared mass transfer and biodegradation rates for
benzene and butanol contaminated gases in HFMBs that utilised dense (latex and
silicone), microporous hydrophobic (polypropylene) and microporous hydrophilic
(polysulfone) membranes. The highest overall pressure drops were observed with the
polypropylene membranes due to the smaller diameter of these fibres compared with
the other fibres. Significant sorption of benzene was observed in initial tests with the
polysulfone membranes; therefore, butanol was used in subsequent experiments with
these membranes. Removal efficiencies for butanol of up to 99% were obtained at an
inlet concentration of 200 ppmv. Dense high permeability latex and silicone
membranes were found to have high benzene mass flux rates, possibly because the
greater solubility of benzene in the polymers than in air creates a greater effective
concentration gradient than observed in the air phase. The low total surface area of
the dense membrane tubes limited overall removal; however, and the polypropylene
168 S. J Ergas
membrane unit was the most effective on the basis of removal per total unit volume
ofreactor.
In my own laboratory we have conducted a number of studies using toluene
as a model VOC. In our first set of experiments (Ergas and McGrath, 1997) a
laboratory scale HFMB was constructed and operated with toluene at varying loading
rates. The gasses pas sed from an inlet manifold to a membrane distributor made from
336 polypropylene hollow fibres (280 flm ID, 63% porosity and active fibre length of
1.1 m). A plot of removal efficiency vs. gas flow rate over the experimental period is
shown in Figure 6.2. Toluene removal efficiencies of gre ater than 97% were
achieved with an inlet toluene concentration of 100 ppmv and gas flow rates less
than 1.0 l/min (l.4 s residence time). When the gas flow rate was increased above 1.2
l/min (1.1 s residence time) a significant decrease in removal effieieney was
observed. Removal efficieney was found to deerease over the four month operational
period due to c10gging of the bioreaetor with microbi al biomass, possibly due to the
growth of nitrifying bacteria.
In subsequent experiments (Ergas el al., 1999) we investigated the effeets of
toluene loading rate, gas residenee time, and liquid phase turbulenee on toluene
removal in a laboratory-scale HFMB. Nitrate was used as a nitrogen souree to
diseourage the growth of nitrifying baeteria. Initial aec1imation of the mierobial
eulture to toluene oeeurred over a period of nine days, after which a 70% removal
efficiency was achieved at an inlet toluene concentration of 200 ppmv and a gas
residence time of l.8 s (elimination capacity of 20 g/m 3 .min). At higher toluene
loading rates a maximum elimination capaeity of 42 g/m 3 min was observed. Liquid
phase reeirculation rate had no effect on toluene removal in the HFMB.
100,--,~,-,--=~~=-------------------,
90
~
o
>-
()
c
Q) 80
·13
it:
w
ro> 70
o
E
Q)
n::
60
Figure 6.2. Removal efficiency in a HFMB vs. gas flow rate (after Ergas and McGrath,
1997). Removal efficiency was determined after an acclimation period at each flow rate.
The inlet toluene concentration was maintained at 100 ppmv, and the liquid recirculation rate
was41/min.
170 S. J Ergas
In biological air pollution control systems, compounds must partition from the gas
phase into the moist biofilm before they can be degraded. Pollutant concentrations at
the gas/biofilm interface can be described by Henry's law:
(6.1)
where H is the Henry's law' s coefficient, Cg is the gas phase concentration, and SL is
the liquid phase concentration. Conventional biofilters have therefore been limited to
the control of relatively soluble compounds. A number of environmentally relevant
compounds such as nitric oxide (NO), hexane and methane are biodegradable but
have high Henry's law constants. For these compounds mass transfer from the gas
phase to the biofilm limits removal unless very large reactor volumes are used.
Owing to their higher mass transfer rates, HFMBs may make biological treatment of
these compounds more economically feasible.
A number of studies have been carried out using propene as a model VOC
because its low solubility makes it difficult to remove in conventional biofilters (air-
water partition coefficient at 2S o C of 8.6). Aflat sheet microporous polypropylene
HFMB inoculated with Xanthobacter Py2 was investigated by Reij et al. (1995).
After five days with an inlet propene concentration of 2300 ppmv, the biofilm
acclimated and 58% propene removal was maintained for the duration of the thirty-
day test. Because ofpropene's poor solubility, all mass transfer resistance was found
to be in the liquid phase. For more soluble compounds, the authors determined that
membrane phase resistance could approach the same order of magnitude as liquid
phase resistance. A similar reactor system and bacterial culture was investigated by
Reij et al. (1997) to degrade propene at concentrations varying from 10 to 1000
ppmv. Once a biofilm was established, propene flux to the membranes was stable,
even at low concentrations (9-30 ppmv) when mass transfer limitations should be
greatest.
Reij and Hartmans (1996) investigated a HFMB that utilised 40
polypropylene hollow fibres with a length of 500 mm, an inner diameter of 1.8 mm
and a pore size of 0.2 Ilm. Propene was again used as a model compound due to its
low solubility. Maximum propene removal rates were 70-110 g/m 3 .h. A gas
residence time of 80 s was required for 95% removal at an inlet propene
concentration of 480 ppmv. The reactor was changed from ammonia as a nitrogen
source to nitrate to discourage the growth of nitrifying bacteria. Increasing the shell
side velocity was found to alleviate clogging of the fibres with biomass. A gradual
Membrane bioreactors 171
4.2 COMETABOLISM
TCE removal. Adding TCE in the gas phase and toluene in the liquid phase resulted
in a maximum TCE removal efficiency of 23%, however, results were highly
variable and appeared to be related to liquid phase toluene utilisation rates and
biofilm thickness.
5. Theoretical models
~:s~~:o~-]
Figure 6.3. Conceptual model ofthe phases ofthe hollow fibre membrane reactor (after
Ergas el al., 1999).
Membrane bioreactors 173
The flux, Jn, of substrate through the membrane can be expressed as:
(6.2)
where km is the membrane mass transfer coefficient, Am is the area of the membrane
in the section, and C n.m is the gas phase concentration on the outcr face of the
membrane.
A number of authors have assumed that gas and membrane resistances are
negligible compared to liquid phase resistance (Ergas and McGrath, 1997; Yang and
Cussler, 1986; Cote et al., 1989) and therefore C n•m is approximately equal to the
concentration in the gas stream, C n-1• Since the membrane is surrounded by biofilm,
the liquid phase concentration at the biofilm interface, Sn,O, can be related to Cn-I
using Henry's law:
Sn,O = Cn _ 1 / H (6.3)
Equation 6.3 sets the inner surface (left-hand) boundary condition for the biofilm
model.
The suspension (liquid volume) was treated as a continuous flow stirred tank reactor
(CFSTR). The mass flux of the substrate, h, from the biofilm to the liquid can be
described by:
(6.4)
where kL is the liquid mass transfer coefficient, Ab is the outer surface area of the
biofilm, SIl.i is the VOC concentration at the outer surface of the biofilm, and SL is
the bulk liquid VOC concentration. Assuming Monod biodegradation kinetics, a
mass balance on the liquid volume yields:
where V is the liquid volume, PL is the biomass density in the liquid, flmax is the
maximum specific growth rate, Y is the yield coefficient, Ks is the half saturation
coefficient, Q is the liquid flow rate, and So is the inf1uent VOC concentrat ion to the
suspension. Substituting Equation 6.4 into 6.5 and solving for Sn,i yields:
(6.6)
This relationship sets the exterior surface (right hand) boundary condition for the
biofilm model.
174 S. J Ergas
(6.7)
where S is the substrate concentration in the biofilm and Ds is the VOC diffusion
coefficient in the biofilm. There is no analytical solution for Equation 6.7 therefore a
numerical solution was generated.
To fit the models, the biofilm density was varied until the predicted removal
matched the observed removal (Ergas el al., 1999). The biofilm biomass density was
calibrated at 29000 mgll, slightly higher than that reported by Characklis and
MarshaU (1990). The numerical model predicted the observed trend that shell side
liquid flow rate, had little effect on observed removal once a biofilm was established.
The model slightly underpredicted the effect that substrate loading rate had on
removal in the system. The only case of poor prediction by the model was the effect
of gas residence time on removal. Observed removals were higher than predicted
removals for these mns. If the pore space of the membranes became water-filled
during the course of experimentation, as discussed above, an added resistance to
mass transfer would be expected, and mass transfer to the biofilm could become
dependent upon the gas flow rate (gas to liquid transfer). Sensitivity analysis
indicated that removal was a strong function of the biofilm phase biomass density
and also of the biofilm diffusion coefficient, with diffusion rates below (lOr9 m2/s
resulting in decreased removal rates.
6. Conclusions
Hollow fibre membrane bioreactors are a promising technology for the treatment of
biodegradable gas phase poUutants. It has been shown to be effective for aerobic
degradation of a range of compounds including ammonia, benzene, butanol,
dicholoromethane, propene, TCE and toluene. Advantages of HFMBs include high
mass transfer rates, low pressure drops and small reactor volume requirements. In
addition, the ability to separate the microbial population from the gases being treated
allows for independent optimisation of each phase of the system. In the opinion of
this author, the most promising areas of air pollution research for HFMBs include:
The greatest disadvantages for the technology are high capital costs and that
it has yet to be demonstrated at fuU scale. Owing to their modular design: however.
HFMBs should be relatively easy to scale up. EnviroGen Inc. and the Medical
University of South Caro lina have developed a prototype with fund ing from the
Membrane hioreactors 175
Department of Energy that they hope to field test in 2001 (Togna, 2000). Long term
studies have been conducted with membrane aeration bioreactors (Stephenson et al.,
2000), which are similar in concept and operation. Membrane reactors have also
been in use for several decades for blood oxygenation (Sikar, 1992) and separation
and retention of biosolids (8rindle and Stephenson, 1996a). In common with
conventional biofilters, HFM8s have problems with excess biofilm growth and long
term stability of VOC degrading biofilms. It is also unknown what effect long
periods of association of membrane materials and biomass will have on mass transfer
rates and mechanical strength in these systems.
Acknowledgements
1 would like to thank my students Ayesha Dolasa, Carolyn Gendron, Yenner Keskiner,
Michael McGrath, Fereshteh Mehmandoust, Andreas Reuss and Leslee Shumway for their
work on these projects. This material is bascd on work supported by the National Sciencc
Foundation. Any opinions, findings, conclusions or recommendations expres sed in this
material are those ofthe authors and do not necessarily reflect the views ofNSF.
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CHAPTER 7 COMBINED ADV ANCED OXIDATION
AND BIODEGRADATION
1. Introduction
In existing biological technologies for waste gas treatment pollutants are transferred
to a water phase and subsequently biodegraded in a biofilm or suspension of micro-
organisms. These two processes impose two important prerequisites on biological gas
treatment: the pollutants should be readily soluble in water and readily
biodegradable. Bioscrubbers, biofilters and biotrickling filters encounter problems
with compounds with dimensionless Henry's Law's coefficients higher than 1 (e.g.,
alkenes, alkanes). In addition, the biological treatment of gases with low
concentrations of compounds with Henry's Law' s coefficients higher than 0.1 (e.g ..
many aromatic hydrocarbons) may be limited by low interphase mass transfer rates
(Groenestijn and Hesselink, 1993). Problems with biodegradability can be caused by
the fact the compounds need anaerobic conditions for their degradation (e,g.,
perchloroethylene) or are only aerobically degraded by co-metabolism (e.g.,
trichloroethylene). Some compounds are in principle biodegradable, but their
elimination in biofilters needs long start up periods. It has been reported that
elimination of certain organo-sulphur compounds only started 5 months after start up
of a biofilter (Cho el al., 1992).
These problems can be solved by a pre-treatment of the waste gas using
advanced oxidation technologies, such as photochemical, photocatalytical, and non-
thermal plasma technologies. This pre-treatment may be carried out in the gas phase
or after absorption, in a water phase. By generating hydroxyl radicals and oxygen
atoms in the gas, hydrophobic compounds can be partly oxidised, which mostly yield
compounds that are more hydrophilic and bettcr biodegradable. Gases with these
partly oxidised compounds can be biologically treated in biofilters or related
equipment at higher volumetric elimination capacities and higher stability than
untreated gases. The combination of a chemical and a biological system is expected
to be more cost efficient than chemi cal oxidation solely, since for a complete
chemi cal oxidation of compounds large amounts of energy are required.
Combined biotreatment and advanced oxidation in water is better known than
that in gases. Complex and recalcitrant compounds in water, such as dyes,
chlorinated hydrocarbons and pesticides can be degraded by photochemical processes
in combination with ozone or hydrogen peroxide, photocatalytical treatment, and
electron beam treatment. It depends on the composition of the water whether
chemical oxidation is used as a pre- or post-treatment in combination with biological
process. If a waste water contains readily biodegradable compounds at higher
concentrations than the recalcitrant compound, it is recommended to start the
treatment process with a biological process, to save energy or chemicals in the
chemi cal process. If the water mainly contains recalcitrant pollutants. chemi cal
oxidation can be the initial operation. A subsequent biological treatment step may be
required because of (1) effluent standards, (2) water reuse and (3) toxicity of products
of advanced oxidation.
179
C. Kennes and M. C. Veiga (eds.), Bioreac/orsfor Was/e Gas Trea/ment, 179-200.
© 2001 Kluwer Academic Publishers.
180 J W van Groeneslijn
Such reasoning can also be made for waste gas treatment. If the gas mainly
contains hydrophobic or poorly biodegradable target compounds, a partial oxidation
by a chemical process should precede a biological process. This sequence can lead to
the lowest costs for near complete mineralisation. If the mentioned compounds
represent only a small part of the target compounds, advanced oxidation may be used
as a post-treatment step. In this post-treatment process complete mineralisation can
be aimed at or only chemical modification (to change the odour properties of
molecules), depending on the specific emission requirements. Even a sequence of
biological treatment, advanced oxidation and a second biological treatment may be
advantageous.
In the sections below important advanced chemical oxidation technologies for
gas treatment are discussed. Almost all studies in this field aim at complete
mineralisation, as the technology is considered to be the sole unit operation to
de grade pollutants in a gas. There are only a few examples of studies which aim at
combinations ofbiological processes with advanced oxidation.
forms of Ti0 2, Degussa P25 has become a research standard due to its wel!-defined
nature and a high photocatalytic activity. Further improvements have been suggested
by using Ti0 2!V205/Pt mixtures (Sanchez et al., 1995).
In most of the gas/solid reactors Ti O2 is present as a coating. Cylindrical flow
reactors are used with Ti0 2 coated on the insi de wal!, while in the middle of the
cylinder a long cylindrical lamp is placed (Sakamoto et al., 1997). They are
alternatively cal!ed annular thin film reactors. The placement of coated bafflcs in the
cylinder may improve the performance (Raissi el al., 1998). Without the catalyst,
these reactors can also be used for photolysis.
Red"ctU
Oxidiser'
e-
k
~~
(9/-
~(I
;:.,
Conductor band 0..,
Photons < 380 nm
E(gap)
Valence bond
Figure 7.1. At the surface of Ti0 2 an electron is liberated by the action of photons. The free
electron and the electron hole both take part in reduction and oxidation reactions.
in the gas phase when photocatalytically oxidising butanol, but at the end, afier
prolonged reaction, only carbon dioxide and water. Oxidation of butylamine yielded
3 intermediates. Vorontsov et al. (1995) found acetaldehyde in the gas phase as an
intermediate product ofthe photocatalytic oxidation of ethanol, and acetaldehyde and
ethylacetate as a result of photocatalytic oxidation of diethyl ether.
Usually the intermediates stay adsorbed onto the catalyst and are further
oxidised. Ameen el al. (1997) revealed that isopropyl a1cohol tirst is adsorbed,
converted into acetone, which may desorbe or may be oxidised to acetaldehyde.
Adsorbed acetaldehyde was rapidly oxidised to acetic acid and further rapidly to
formaldehyde and formic acid, then slowly to carbon dioxide. The presence of
acetone in the gas phase during the photocatalytic oxidation of isopropyl alcohol was
earlier demonstrated by Ameen and collaborators (1995).
The higher solubility of intermediates was positive1y used in a process
developed by De1prat et al. (1997) in which an air flow containing 2J-dimethyl
pyrazine passed a Ti0 2 suspension in water, irradiated with 340 nm UV waves. 2,3-
dimethyl pyrazine, an odorous compound produced by food processing, was
eliminated from the gas phase, while (intermediate) products were retained in the
water phase. Fourteen products were identitied. Organic nitrogen was transformed
into ammonium ions, which were very slowly oxidised into nitrate ions.
2.2.4. Kinetics
The economy and space requirement of photocatalytic reactors in industrial
applications depend on the required gas residence time, which depends in turn on the
degradation rate of the target compounds. The rate of degradation of volatile
compounds in photocatalytic reactors with Ti0 2 as the catalyst depends on the light
intensity, the available surface area of Ti0 2, the concentration of the target
compound, the water vapour concentration, the oxygen concentration and the nature
ofthe compound.
Many researchers have found satisfactory removal efticiencies in photo-
reactors using gas residence times of a few seconds. Graf el al. (1997) were able to
eliminate ethylene down to a level of 50 ppbv within 1 to 3 seconds. Another study
indicated that more than 99% photocatalytic conversion of PCE could take place in
0.5-2 seconds. The degradation rate appeared to be directly proportional to the light
184 J. W van Groeneslijn
intensity to the power 1.2 and water vapour inhibited degradation (Hung and Yuan,
1998). Humidity appears to be important: Li et al. (1997) demonstrated that the effect
of water vapour depends on the nature of the compound. The conversion of PCE
might be inhibited by water vapour, but the oxidation of toluene was stimulated by
increasing relative humidities in the range 0-10%. Higher humidities did not have an
additional stimulating effect. According to the authors these different effects of
humidity on the conversion of toluene and PCE imply that thcir photocatalytic
oxidation mechanisms are different. The photocatalytic oxidation of toluene may be
through hydroxyl free radicals, which needs water molecules to initiate, while for
PCE the oxidation mechanism may be through chlorine free radicals, which does not
need water molecules. The water molecules can be adsorbed onto the Ti0 2 surface
and therefore block the oxidation reaction.
Lichtin and Sadeghi (1997) studied the effect of VOC concentration on the
degradation rate, using benzene as a model compound in the range of 90-12000
ppmv. First order kinetics were found: the rate of initial oxidation of benzene was
directly proportional with its concentration. In their test equipment the initial
oxidation took minutes, while the CO 2 production approached completeness in more
than 1 hour. This indicates the accumulation of intermediate compounds and
demonstrates that partial oxidation may be economically more attractive than
complcte oxidation. The same study revealed the independence of initial benzene
oxidation on O2 concentrations between 0% and 100%, and the increase of CO 2
production rate with increasing 02 concentrations. Sakamoto el al. (1997) a1so found
first order kinetics for toluene in the 200-1200 ppbv range. The removal of toluene
was always 75%, independently on the toluene concentration. As expected, the
removal efficiency was dependent on the catalyst surface area and the gas flow rate
through the reactor. Although first order kinetics is common in gas phase
photocatalysis, exceptions exist. Photocatalytic oxidation of isopropy1 alcohol shows
first order kinetics up to concentrations of 40 ppmv, but near independence was
found at concentrations above 60 ppmv (Ameen et al., 1995). This behaviour
supports Langmuir-Hinse1wood kinetics.
The effect of light intensity was studied in a detai1ed way using TCE as a
model compound (Upadhya and Ollis, 1998). At high concentration ranges (1000
ppmv) the amount of VOC converted per g Ti0 2 per minute appeared to be directly
proportional to light intensity in a linear dependency, but in such way that low light
intensities were more efficient. At low concentrations (60 ppmv) such linear relation
could not be found.
alkenes react faster than homologue alcohols. The same posltlve correlation of
reaction rate and molecular weight was found for these chemical classes. A same
effect was found for non-oxygenated (real hydrocarbon) aromatic compounds. The
addition of one or more hydroxyl groups to a molecule makes aromatic compounds
more reactive with hydroxyl radicals. For instance, phenol is 20 times more reactive
than benzene. This means that the accumulation of such oxidation intermediates is
unlikely. Neverthe1ess, phenol can be detected during photochemical oxidation of
benzene, while benzaldehyde, o-cresol, m-cresol and p-cresol can be measured as
products from toluene oxidation and photochemical conversion of o-xylene produces
o-tolualdehyde, 2,3-dimethylphenol and 3,4-dimethylphenol.
A few researchers combine photocatalysis and photolysis. They use UV
radiation with a relative high wavelength, Ti02 as catalyst and addition of ozone to
promote indirect photolysis and to prevent catalyst deactivation. Ozone can be
produced in situ or by remote ozone generators. Alberici and Jardim (1998)
investigated gas-phase photocatalytic oxidation of different classes of VOCs,
including alkanes, ketones, a1cohols, chlorinated compounds and aromatic
compounds, using an annular thin film reactor with a black light lamp (maximum
radiation at 365 nm) and Ti0 2 as catalyst. For all organic compounds tested, catalytic
deactivation was not observed, except for toluene. Co-injection of ozone could
prevent this deactivation. The addition of ozone had only clear advantages for
toluene (to prevent deactivation) and for pyridine. The destruction of 620 ppmv
pyridine was increased from 16 to 68% by addition of 1 mg 0 3/1 air, produced by a
high voltage ozone generator. Similar experiences of increased elimination rates by
addition of ozone in photocatalytic reactors can be found in Obee and Hay (1997)
and Ollis (1995).
Other researchers combine photolysis and high temperatures: the photo-
thermal process. Chen et al. (1997a) proved that at 600 °C BTEX mixtures could be
treated within 10 seconds in a reactor with UV radiation with a wave1ength of 185
and 254 nm. 62%, 87%,94% and 96% destruction was observed ofbenzene, toluene,
ethylbenzene and xylene respectively.
A plasma is a mixture of free moving electrons and positively charged ions. It can be
generated in a medium between two electrodes. It already can be produced if a high
voltage AC (10-30 kV) is applied for a very short time (1-10 milliseconds). During
these short pulses the medium will not be heated, but the plasma is nevertheless
produced. It is called a non-thermal plasma. If the electricity pulses are too long, the
medium acts as a conductor and is substantially heated. As a result high energy costs
are involved. Non-thermal plasmas are an excellent source of gas-phase free radica1s
(O, OH and H) and other active species useful for destroying pollutants (Cal and
Schluep, 2000). Therefore non-thermal p1asmas are the logic option for gas
treatment. They can be generated by die1ectric barrier discharge (DBD), corona
discharge or an e1ectron beam.
According to Cal and Schluep (2000) using non-thermal plasmas for gas-
phase pollution control shows much promise, but is still in its early stages of research
and development.
Combined oxidation-biodegradation 187
Table 7.1. Comparison of energy use by different processes for 90 % removal of VOCs
from dilute waste gases (1 g VOC/m 3)
different specific rate. This implies that for mixtures of pollutants in air a high energy
use and long gas residence time may be required ta treat the gas according ta
emis sion standards. The design of the system will be most dependent an the
compound with lowest reaction rate. In this respect it may bc interesting again ta
study a possible complimentarity between oxidation in non-thermal plasmas and
biological processes with respect to the ease ta oxidise different classes of VOCs.
Inorganic compounds can also be oxidised in non-thermal plasmas produced
by DBD. Double dielectric barrier discharge has been demonstrated effective at
oxidising NO into N02 and HN0 3 (Federle et al .. 1997). The much higher solubility
of the products in water made it possible to treat the gas with a more conventional
gas treatment system: a horizontal wet scrubber utilising hydrogen peroxide and
sodium hydroxide to absorb the products and convert them to nitrate salts. The
authors did not consider a biological post treatment system, but it is expected that an
absorber and denitrification re actor may be an interesting option to treat these gases
with NO (e.g. fiue gases). The authors developed the system for diesel-powered
generators and found a NO x elimination efficiency greater than 70%. The NO
conversion efficiency was 17 eV per NO molecule oxidised and the overall system
efficiency was 40 eV per NO x molecule removed. The power consumption of the
N Ox removal process was estimated to be less than 10% of the total power produced
by the generator.
Slightly different results were found by Yang el al. (1997): 130 ppmv NO in
air was converted into N2, O2 and N0 2 (not HN0 3 !) in packed beds with dielectric
materials (barium titanate) in which non-thermal plasmas were produced by electric
discharges. The 40 ppmv N0 2 produced from 130 ppmv NO was furthcr removed
from the gas phase in a post treatment step Ca caustic wet scrubber).
A humid waste gas containing S02 and NH 3 can be cleaned within 2 - 6
seconds in a re actor with pulsed corona discharge. In such reactor particles of
(NH4)2S04 were produced (Chang and Choi, 1998). Another study describes the
conversion of S02 in fiue gas into S03, which precipitate onto the fiy ash (Amirov et
al., 1995). The authors found that the presence of particles in the gas phase
stimulated the reaction efficiency and that the addition of water vapour reduced the
energy costs. One Wh is required ta remove 12 ppmv from one Nm 3 flue gas. A
small pul sed corona streamer pilot plant for 200 Nm 1 flue gas per hour was tested by
Mattachini et al. (1995). A gas residence time of 0.6-0.7 s seemed to be sufficient.
The e1ectron beam technology is based on an electron gun that shoots high energetic
electrons to a target object. The electron gun comprises an electron source, i.e .. a
glow cathode, and an acceleration part that gives the electron a high speed
(comparable with a TV or an electron microscope). The electron gun, or EB (electron
beam) generator, is made vacuum to avoid hindrance of electron movement. The
electrons leave the EB generator via a window, made of thin but solid material, e.g.,
aluminium or titanium foiI. By interaction and collision with matter on their pathway,
the high-energetic electrons generate a multitude of exited molecules. X-rays are a
secondary effect of electron beam discharge. This secondary radiation creates
re active species as well, but also requires specific safety measures connected to this
technology.
190 J W van Groeneslijn
The number of studies on advanced oxidation technologies in water is larger than that
in gases. AlI technologies described above can be applied in a water phase. In water
treatment, the combination with biological technologies is considered more
frequent!y.
In 1994 the Dutch Government has made an overview on the possibilities of
chemi cal oxidation technologies for water treatment. A broad view on the effects of
such treatment was presented, e.g., the changed eco-toxicology of water and the
changed BOD/COD ratio, anticipating on biological post-treatment. In this study the
advanced oxidation technologies were only represented by photochemical processes
Combined oxidalion-biodegradation 191
benzaldehyde and traces of benzoic acid. Interestingly, the reaction continued in the
effluent gas collection vessel outside the photochemical reactor. Probably radicals
and instable intermediates produced in the UV reactor stiU reacted with styrene after
leaving the reactor. This not -optimi sed reactor system consumed 15 k Wh per 1000
m 3 gas containing 100 mg styrene/m 3 and oxidised styrene for 80%. This high energy
consumption may be lower after optimisation ofthe photochemical reactor.
Besides photolysis also photocatalalysis was studied. For this purpose a
closed system was used with a gas recycling loop and a reactor with a Ti0 2 coating
and a UV lamp. Styrene was only eliminated if both the UV light and Ti0 2 were
present in the reactor. Immediately after the UV irradiation was started styrene
disappeared, while CO 2 was only slowly released over a period of 135 minutes. As
expected, eventually 8 moi CO 2 were produced per moi eliminated styrene. This
means that complete oxidation takes a lot oftime and energy.
To prove that products from partial oxidation of styrene can be converted in
biofilters faster than styrene, laboratory scale biofilters filled with compost were
tested with different gases containing one organic poUutant: styrene, benzaldehyde,
acetophenone or I-phenylethanol. The elimination capacities found after sufficient
adaptation time can be found in Table 9.2.
Abbreviations
Acknowledgements
The author gratefully acknowledges Jan WilIem Assink and Hennan Kok for advices and information
on advanced oxidation technologies. This chapter was written with support from TNO Environment,
Energy and Process Innovation, Apeldoorn, the Netherlands.
Combined oxidation-biodegradation 195
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CHAPTER 8 ROTATING BIOLOGICAL CONTACTORS
1. Introduction
Waste gases are found in alI branches of industries. As long as the contents of
organic or inorganic substances are be10w local admissible values the waste gas may
be released to the environment without any additional treatment. If these specific
values are higher the waste air shall be treated before leaving the plant site. Clearly
gaseous wastes are difficult to store; therefore most of the waste must be cleaned in
place where it is generated mostly by fast chemical absorption, adsorption or
incineration (see Chapter 2). Industries like to be flexible in producing products.
Therefore variable waste production may also be observed. AlI biological waste gas
systems are extremely well suited for constant gas loads and constant waste
composition which is not the standard case. Normally the loads and contents of
organic by-product in waste gases is changing within short periods of time. This
explains why only few systems are incorporated in industrial applications. However,
many different approaches have been attempted to overcome the load fluctuations.
The RBC was originally deve10ped for waste water streams as an alternative
to standard sewage systems. Several discs -acting as biofilm carrier- are mounted on
a shaft at defined distances from each other. The discs are rotating at a speed of about
two revolutions per minute in order to increase mass transfer and to control the
biofilm thickness by the shear force induced between the biofilm and the waste
water. Charaklis (1990) has divided the growth of the biomass on inert carriers (here
discs) in eight steps:
biofilm detachment rate is equal to its growth rate. This may ideally be realised in a
rotating system with fixed carriers.
The idea of RBCs in waste water treatment goes back to the beginning of the
tewntieth century. Tests were performed in Germany and in the USA between 1920
and 1930, but the idea did not spread out. In 1950 the RBC was further developed at
the University of Stuttgart in Germany. The first industrial system was built in 1960
(Antoine, 1976). Because of a very poor construction the shaft of this first RBC
broke down. Furthermore the discs on that shaft were unsufficiently fixed. The
rumors about these problems were not very favorable for further introduction of the
system (Andowski, 1956).
The carrier discs were fixed vertically to the horizontaJly mounted and
rotating shaft. The waste water entered on one side of the mostly covered part of the
reactor and flew from one cell to the next one. Each cell contained two discs. The
mean residence time was very short compared to conventional sewage plants. In
other constructions curved PVC sheets have been used, winding them around the
shaft like a big cylinder. The flow of the waste water is in such case paralle1 to the
shaft. Depending on the design, between 40 and 60% of the volume of the carrier is
immersed in the liquid. During the rotation the biofilm ahsorbs the oxygen in the gas
phase (upper part) and the organic material in the liquid phase. The rotation leads to
a good mixing and holds detached biofilm particles in a floating condition (Antoine,
1976). In the fie1d of waste water treatment RBCs are considered to present the
foJlowing advantages (Bitton, 1994):
A similar problem occurs in biological waste gas treatment systems as in waste water
systems, Le., the accumulation of biomass leading to clogging phenomena. A
Canadian GrOUpl (Kahler and McKim, 1989) reported on the use of a rotating system
for waste gas treatment. Our group at ETH (Ruediger, 1999) concluded experimental
tests and has adapted RBC systems since 1997. Sabo and Fischer (1996) reported
about a rotating biofilter. The goal of their investigations was to improve the wetting
of the biomaterial and to decrease the tendency of compression of the filter material.
There is only limited experience with this kind of reactor. The above mentioned
group performed tests in a pilot plant with phenol during 373 days. For gas feed
concentrations between 1 and 7 g/m3 the removal efficiency remained above 99.9 %.
Our group wanted to investigate this novel system and carried out tests under defined
conditions. The Canadian group2 kindly provided parts of the pilot facility. The pilot
facility (Figure 8.1) consisted ofthree parts:
Figure 8.1. Process diagram of an RBC pilot facility (RBC with four chambers) (Ruediger,
1999).
2 ibid.
204 Ph. Rudolf von Rohr and P. Ruediger
The reactor consisted of a cylindrical outer shell with several windows and an
inner shaft with several carrier discs fixed on it. The diameter of each disc was 28
cm. The distance between each disc was 10 mm. The shaft could rotate at variable
speeds between 5.8 and 8.8 rpm. The liquid container was conditioned with sodium
hydroxide (NaOH) and specific nutrients. Furthermore the temperature was
maintained at 30° C. The main parameters are summarised below:
The results are presented using the performance parameters defined below. Some of
these parameters are similar as for biofilters and have been extensively defined
previously (Chapter 3):
Elimination capacity:
(8.1)
Removal efficiency:
RE 100 (8.2)
VG (c GO - c G•ou' ) EC (8.3)
SEC =
a VR a
SLO = (8.4)
Data on elimination capacity (EC) and removal efficiency (RE) are shown in
Figure 8.2.
Rotating Biological Contactor 205
140 I I
120 f- t, O
I O
O -
100 f- t, O -
~ t,
-
1
O
80 l-
60 l- t, <> <> OO
~t,<>t, <El
~
O
-
w -
40 1-
20 i/fS)<> O
O
-
O
100
80
~
~ 60 O
<> o O
w 40 $> O O O
D:: O
~~t,oMO °t,O O
O
20 <> <> t, t, O
V G
<>
O
O 5 10 15 20
eoo [g/m'1
• Mass transfer of oxygen and dichloromethane into the liquid phase is increased;
206 Ph. Rudolf von Rohr and P. Ruediger
• The amount of liquid increases on the discs whereby the mass transfer from the
gas phase into the liquid decreases. The rate of absorption increases;
• The liquid is better mixed. Oxygen and the pollutant are better distributed in the
reactor;
• Energy consumption increases;
• Bad mixing is observed. Detached parts of the biofilm sediment to the reactor
floor and anaerobic zones appear;
• The uptake of oxygen is decreased;
• The shear forces on the biofilm decrease;
• The release of the non-volatile components from the biofilm is hindered. They
may accumulate eventually leading to inhibition ofthe activity ofthe biofilm.
In the following section, the degradation capacity of the rotating biofilm reactor will
be compared to that of biological trickling filters. The DCM biodegradation data
from Diks (1995) and from Zuber (1995) will be used for comparison. In order to
make a valid comparison, geometrical and operational values must be considered.
These data are presented in Tables 8.1 and 8.2.
35
o
30
o
o
25 v
o O c Go =42 g/m 3
~ 20 o o c Go =16.1 g/m 3
UJ r.
c:: 15
D D D o D
10 D
D
5
o
O 2 4 6 8 10
n [rpm]
Figure 8.3. Influence ofthe rotational speed on the removal efficiency (RE) of the described
rotating biological contactor. Substrate: dichloromethane in air; gas flow rate: V G = 60.7
I/min.
Rotating Biological Contactor 207
Table 8.1. Geometrical variables ofbiotrickling filters and RBC for the removal of DCM
A VR Atot, dK AK L Type of References
m2/m l 1 m- m 10·3 m' m packing
750 339 254 0.4 125.6 2.7 y," ceramic Diks,1995
Novalox-
saddle
350 7.6 2.66 0.096 7.28 1.05 Mellapak Zuber, 1995
350.Y
87 85.74 7.44 0.312 76.45 1.112 Discs RBC for waste
air
Table 8.2. Operational data ofbiotrickling filters and RBC for the removal ofDCM
vG tG b T cGO,max LO ma• EC max References
m/h s m3/m 2 .h ec glm 3 glmR3 .h glm/.h
160 61 3.6 20 Il 650 157 Diks,1995
160 23.6 II 30 20 3051 420 Zuber, 1995
18.4- 71.3- n = 5.8 rpm 30 17 858 120 RBC for
65.1 218 waste air
0.5 2
"
6 6 1-
0.4
1,5
:c- :c- 6
6
E NE
~.~
,
0.3 6
:2! :2!
()
w
cn 0.2 In
• D ()
w
cn
if!J [ [] •
O 0,5
6Î
0.1 w O ~
~DD
o o
O 0.2 0.4 0.6 0.8 O 4 8 12 16
SLO [g/m'.h] SLO [g/m'.h]
Figure 8.4. Comparison of dichloromethane removal from the gas phase in biotrickling
filters and in a rotating biological contactoT. (Diks, 1995; Zuber, 1995; Ruediger, 1999).
208 Ph. Rudalf van Rahr and P Ruediger
With a surface-specific load of less than 1 g/m 2 h, the performance values for
the rotating biofilm reactor were lower than those obtained by Zuber (1995) and
equivalent to values in the upper range of those measured by Diks (1995). This
characteristic is found even though the part of the rotating biofilm re actor submerged
in the liquid phase, which would be expected to have a greater resistance to diffusion
than the unsubmerged part, was inc1uded in the calculations of the surface-specific
elimination capacity. Comparison with the data from the literature showed that the
part ofthe biofilm covered with the liquid phase as well as the biomass suspended in
the liquid phase can contribute to biodegradation. An increased biomass activity in
the rotating biological contactor is less probable because all reactors were inoculated
with microorganisms especially adapted to DCM, namely DMI and DM2.
At higher loads, those gre ater than approximately 4 g/m 2 h, the values from
Zubcr (1995) level off, indicating an increasing limitation of the reaction. In contrast,
the values for the RBC continue to increase. Therefore the degradation capacity of
the rotating biological contactor was limited by diffusion even at high loads.
In the present section differences between short term and long term influences on the
elimination capacity will be considered. Long term influenccs are paramcters
influencing the structure and the activity of the biofilm. These influences determine
the maximum performance of the RBC plant. Long term influences are assumed to
take place on a time scale of several days or weeks. Short term influences affect only
the combined diffusion and degradation. In the lattcr case the characteristics of the
biofilm are considered to remain unchanged. Short term influences have a time scale
of minutes. Parameters such as the number of revolutions per minute and substrate
concentrations can present both short term and long term effects on the degradation
capacity of an RBC. Parameters as pH, temperature, and nutrient or salt
concentrations, which have both short and long term influences, are assumed to
remain constant.
surface-specffic Ioa<!
liquid bulk
• Waste gas flows through the gas filled space in the re actor;
• The largest part ofthe liquid phase (the bulk fluid) is collected in the lower part of
the reactor;
• The rotation ofthe discs lifts liquid from the bulk fluid up into the gas-filled area.
This liquid interacts with the biofilm. To simplify the model one could regard this
liquid as a film adhering to the biofilm;
• The biofilm.
In the short term the rotational speed and the substrate load int1uence
diffusion in the reactor and the kinetics of biological degradation. The measurements
presented above examine these short term phenomena.
The substances can be absorbed from the gas phase either by the liquid film
adhering to the biofilm or by the bulk liquid. Because of the rotation of the discs a
constant transfer between the liquid adhering to the biofilm and the bulk liquid
occurs.
In their model of the dependence of the distribution of a liquid on a disc in a
RBC Vaidya and Pangarkar (1987) used the following parameters: disc rotational
speed; distance from the centre of the disc; viscosity and surface tension of the
liquid, and the extent to which the discs were immersed. In the model it was assumed
that the liquid remained attached to the disc. The movement of the liquid relative to
the disc while it is in the gas phase was ignored. Using the time periods during which
the individual points on the disc remained in the gas phase, the concentration profile
could be determined. Using such a profile, absorption rates and, in the end, substance
transfer coefficients could be calculated. According to these calculations. the mass
transfer coefficient for a disc half immersed in the liquid phase depends solely on the
rotational speed. The interaction between the biofilm and the liquid was not
discussed.
In practice it must be assumed that the t1uid moves relatively to the disc. The
extent to which this t10w contributes to the total absorption rate should be further
investigated.
Owing to the rotation of the disc the oxygen concentration in the biofilm
varies. In the gas filled space the biofilm adsorbs oxygen from the gas phase. Thus
oxygen concentration in the biofilm increases. On the submerged part of the disc thc
oxygen concentration in the biofilm decreases. Gujer and Boller (1990) created a
model that also considered anaerobic biodegradation of organic substances, flake
formation, and shear-rate-dependent detachment ofthe biofilm. Modelling of oxygen
diffusion into the liquid was of great interest. In this model the fluid taken from the
bulk liquid within the biofilm was ignored. Oxygen from the air was assumed to be
transfered directly from the gas phase to the biofilm. Factorial analysis was applied
to the variations in oxygen concentrations within the biofilm resulting from disc
rotation. The period of exposure of the biofilm in the gas filled area was too short to
seriously influence the oxygen concentration profile caused by the biological
degradation. Only at small angular velocities did the increased exposure time re suit
in an increased penetration depth. Gujer and Boller (1990) concluded that the
influence of disc rotation on the degradation capacity of the biofilm must be taken
into account only at very small rotational speeds. In their model they did not
differentiate between diffusion into the liquid film and diffusion into the bulk liquid,
but used instead an average kLa value.
Rotating Biological Contactor 2]]
limited by
mass transfer.
independent of
rotation speed
limited by reaction
Iimited by
mass transfer,
dependent of
rotation speed
substrate load
Figure 8.7. Regimes dependent on the rotationa! speed and the substrate load for constant
biofilm conditions.
3. Design improvements
In the experimental RBC the gas phase f1ew tangentially along the discs (Figure 8.8).
For such construction, different residence times re suit for the gas molecules in the
reactive part of the RBC. Therefore it was suggested feeding the gas into the re actor
through slots in a hollow shaft. Such construction forced the waste gas to f10w in a
radial direction with respect to the discs.
212 Ph. Rudal( van Rohr and P. Ruediger
Central introduction of the gas phase would also make it possible to use a
packing instead of discs as support for the biofilm. For this purpose the packing
could be held in the shape of a drum by a wide meshed screen. The extent to which
the packing would hinder removal of detached biofilm pieces must still be
investigated. Preliminary results obtained with a similar construction as the RBC
(hollow shaft) showed quite high removal efficiencies of toluene (Vinage el al ..
2001). Fora flow rate of 1 m 3/h with a high concentration of3.1 g/m 3 , the removal in
the RBC was 1.9 g/h. Referring to the active biofilm in the used re actor, the surface-
specific elimination capacity was 0.37 g/m 2.h.
4. Conclusions
The RBC is an alternative technology to other biological waste gas trcatment systcms
for low loaded waste gas flows. Simple design, flexibility, and good elimination
capacity are some ofthe highlights.
Further theorctical and experimental work is needed to check long term
stability and to define scaling up criteria. Industrial experience will be necessary to
set up a simple automation system and to test the constructional parts, corrosion
problems, its adaptation to different pollutants in a practical environment and to
confirm scale-up criteria and theoretical predictions.
The combination with other physical or chemical waste gas treatments (like
adsorption or chemi cal oxidation) may be necessary to overcome the two major
drawbacks Iinked to biological waste gas treatment systems, namely the long
adaptation time of the microorganisms and the limited degradation. However,
biological waste gas treatment systems are easy to handle and seem to require only
minimalmaintenance. Therefore they are interesting for further investigations.
Rotating Biological Contactor 213
Symbols
a m 2/m 1 specific diffusion surface
Atot m2 total diffusion surface
A m2 diffusion surface
AK m2 cross-sectional area ofthe column
b m1/m 2 .h sprinkling rate
CGO,max kglm 1 maximum concentration at gas entry
dK m column diameter
dSoh m disc diameter
EC g/m1.h eliminatiOl1 capacity
EC max glm1.h maximum eliminatiOl1 capacity
kLa Ils mass transfer coefficient
L m reactor length
LO glm'.h load
LOmax glm 3 h maximum load
n rpm shaft speed
RE % removal efficiency
SEC g/m 2 h surface-specific eliminatiOl1 rate
SLO g/m 2.h surface-specific load
T ec temperature
tG s mean hydraulic holdup time for the gas phase
VG m1/s volumetric gas flow
VI ml/s volumetric liquid flow
VR 1 reactor volume
m
VG m/s superficial gas velocity
Refcrcnces
Andowski, L. 1996. Past, present and future ofthe RBC industry. Water Eng. Manage. 143: 31-34.
Antoine, R.L. 1976. Fixed biological surfaces-wastewater treatment; the rotating biological contactoL
CRC Press Inc., Cleveland, Ohio.
Bitton, G. 1994. Wastewater microbiology. Wiley Series in Ecological and Applied Microbiology,
Wiley-Liss., New York.
Boumansour, B.E. and Vasel, J.L. 1998. New tracer gas method to measure oxygen transfer and
enhancement factor on RBC. Water Res. 32: 1049-1058.
Characklis, W.G. and Marshall, K.c. 1990. Biofilms. J. Wiley & Sons, Inc., New York.
Diks, R.M.M. 1995. Ph.D. thesis, Technische Universiteit Eindhoven, The Netherlands.
Gujer, W. and Boller, M. 1990. A mathematical model for rotating biological contactors. Wat. Sci
Technol. 22: 53-73.
Heits, H., Laurenzis, A. and Werner, U. 1997. Biologische Abgasreinigung mit kontrolliertem
Biomasseaustrag im periodisch rlickgesplilten Rieselbettreaktor. Gefahrstoffe Reinhaltung der Luft.
57: 153-158.
Kahler, B.D. and McKim, M.P. 1989. Biological contact gas scrubber for waste gas purification.
Ontario Research Foundation, Canada.
214 Ph. Rudalf van Rahr and P. Ruediger
Lu, c., Li Hung, c., Lee Lian, Y. and Lin Min, R. 1997. Effects of disc rotational speed and
submergence on the perfonnance on an anaerobic rotating biological contactor. Environment Internat.
23: 253-263.
Peyton, B.M., Charaklis, W.G. 1993. A statistical analysis of the effect of substrate utilization and
shear stress on the kinetics ofbiofilm detachement. Biotechnol. Bioeng. 41: 728-735.
Sabo, F. and Fischer, K. 1996. Entwicklung und Erprobung eines neuartigen Rotor-Biofilters. In:
Fortschritte bei der thermischen, katalytischen, sorptiven und biologischen Abgasreinigung.
Kommission Reinhaltung der Luft im VDI und DIN (ed.). VDI Verlag, Diisseldorf, pp. 559-565.
Sassi, G., Ruggeri, B., Bosco, F. and Specchia, V. 1996. Relaxation time analysis of a rotating
biological contactor. Chem. Engin. Sci. 51: 2853-2858.
Stewart, P.S. 1993. Model ofbiofilm detachement. Biotechnol. Bioeng. 41: 111-117.
Vaidya, R.N. and Pangarkar, V.G. 1987. Convective diffusion model for mass transfer in a rotating
biological contactor: disc submergence less than 50%. Water. Res. 21: 1499-1503.
Vinage, 1., Wegmann, A., and Rudolf von Rohr, Ph. 2001. Novel reactor for waste gas purification:
Modified Rotating Biological Contactor. In: Proceedings ofthe 94'1> Annual Meeting & Exhibition of
the Air & Waste Manage. Assoc., 2001, Orlando, FL.
Ange1a R. BIELEFELDT
1. Overview
in the liquid suspension primarily in the second re actor. This two-reactor system is
more expensive because of having multiple reactors. In addition, biomass plugging
of spray units and attached biogrowth in the first stage are difficult to control.
This chapter summarises the pertinent design factors for the general category
of activated sludge reactors. Differences in the various sub-types of reactors are
described. Fundamentals of mass transfer and biodegradation are incorporated into a
model to aid the design of suspended growth gas treatment reactors. Published
applications of suspended growth reactors to treat various contaminants are
summarised. Finally, the costs of using activatcd sludge systems to treat
contaminated gases are discussed.
2. Process description
In true activated sludge treatment the primary function of the re actor is to treat
dissolved contaminants in waste water. The re actor has generally been optimised for
biodegradation of the contaminants in the liquid. Gas is introduced into the reactor to
provide oxygen as an electron acceptor allowing suspended aerobic bacteria to
degrade dissolved organic contaminants. Mass transfer considerations in thc design
of these reactors are generally focused on oxygen delivery aud mixing. Current
application of activated sludge reactors to treating contaminated gases has required
little, if any, modification of the waste water treatment basins. The contaminated air
is simply used in addition to, or in place of, the clean air commonly used to supply
oxygen. A diagram showing the major components of activated sludge treatment
systems is shown in Figure 9.1.
Activated sludge is a very common process used to treat municipal wastc
water and industrial process wastewaters. The organic contaminants in municipal
waste water are generally readily biodegradable and have a high oxygen demand.
The waste water flows into a tank where suspended bacteria de grade the organic
compounds and/or transform inorganic compounds (i.e., ammonia to nitrate). To
supply sufficient oxygen to the bacteria, aerators with good mass transfer
characteristics are installed in the tank.
Most activated sludge systems supply the oxygen that is required via diffused
air. Altematives to air diffusion are pure oxygen diffusion or l11echanical surface
aeration. The diffuser placel11ent and gas tlow rates used for aeration are generally
sufficient to provide l11ixing of the liquid and to l11aintain the bacteria in suspension
(greater than 3 std Cl11 3 airlcl112 basin floor area.min, recol11l11ended by Metcalf &
Eddy, 1991). There are a limited number of cases where both submerged diffusers
and mechanical mixers are used to achieve desired levels of mixing and oxygen.
The two most commonly used types of diffused aerators are: (1) porous or
fine bubble diffusers; and (2) non-porous or coarse bubble diffusers. The porous
diffusers are generally made of ceramics in the form of plates or individual domes;
Activated Sludge 217
Irealed gas
o o 4-Bm
o o o Iiquid
risinggas o
depth
o bubbles o
o o o o Irealed
waslewaler
t
b '!>C t r i ~ I o waslewaler
suspenslo9J o
filter o o o
II...!:C:2.0n!!!l:!!!am~in~al~e.9.d+lCJa~ir~dlliiff~U~S@io~n:gd~ev~ice~==:Jl
tr_ o-o
o
\
gas
- - - - ----- i
"
moislure blower I activaled slud~)
+ - - - - seltled
- - -biomass
- - -(relurn
---
~ ~,
biomass ~
they are altematively made of membrane material on a plate, disc, or tube. As air is
forced through the porous diffuser material it enters the liquid in the form of tiny gas
bubbles typically ranging in diameter from 1 to 4 mm. Non-porous diffusers
generally consist of small holes in pipes or plates produc ing large gas bubbles of 6 to
10 mm diameter in the liquid. Smaller gas bubbles result in higher mass transfer
efficiency because greater contact area between the gas and liquid allows diffusion of
the gas molecules into the liquid. Therefore porous diffusers are generally superior to
coarse bubble aerators. Despite gre ater headloss of air inside fine bubble diffusers
(greater than 5 cm of water head) versus coarse bubble aerators, fine bubble diffusers
have still been shown to cost up to 50% less to aerate an activated sludge system
treating municipal waste water (US EPA, 1989).
Clogging of the porous diffusers can occur due to particulates in the inlet gas
and bacterial growth on the surface of the diffuser. Filtration of the gas prior to the
inlet manifold of the activated sludge tank is frequently used to prevent c10gging of
porous diffusers. Gas filtration is not required for coarse bubble aeration. Excessive
bacterial growth on the surface of the diffusers in contact with the water can occur
with either type of aeration device. The bacterial growth increases the headloss
across the diffuser and may change the aeration characteristics in the basin. This
fouling effect will decrease the aeration efficiency over time. Fouling can be detected
operationally by an increased blower discharge pressure and/or coarser bubbles. To
alleviate the effects of bacterial fouling, it is recommended that porous diffusers be
routinely c1eaned. Ceramic diffusers can be c1eaned by draining the basin and using
an aggressive water spray (fire hose) or by immersion of the diffuser heads in an
acidic solution. For membrane systems, a burst of higher airflow may dislodge
attached bacteria.
Manufacturers traditionally report the characteristics of their diffuser devices
as a specific oxygen transfer efficiency (SOTE) at a given submersion depth of the
diffuser and gas flow rate. The number of diffusers located in the tank is selected to
provide the desired mass loading of oxygen to the system and typically ranges from 1
to 7/m2 (US EPA, 1989; Metcalf & Eddy, 1991).
Activated sludge tanks are generally concrete basins that are 4.5 to 7.6 m
deep with a width to depth ratio of 1 to 2.2 : 1 to allow good mixing characteristics of
218 A.R. Bielefeldt
the water (Metcalf & Eddy, 1991). The total biomass concentration in the reactor
generally ranges from 2000 to 5000 mg/L These high biomass concentrations are
maintained in conventional activated sludge systems by operating with a longer
biomass retention time (SRT; 5-10 days) than hydraulic residence time (HRT; 5 to
10 h). A elarifier generally follows the aeration basin to settle out the biomass in the
waste water. The concentrated biomass settled at the bottom of the elarifier is
recyeled to the aeration bas in (return activated sludge). A selected portion of this
biomass is also wasted as sludge or untreated biosolids rather than being returned to
the aeration basin. If hydrophobic contaminants present in the gas are treated in an
aeration basin, adsorption to biosolids may aid gas treatment. Note that in studies
where contaminated gas has been treated in full-scale activated sludge tanks, the tank
dimensions and mass transfer characteristics for the gas injection have generally not
been reported in detaiL
Although there is a high concentration of bacteria in activated sludge tanks, a
significant portion of the suspended biomass may not be actively degrading the gas-
phase contaminants. Therefore, care must be taken if the total biomass is used to
predict reactor performance. A study with synthetic organic compounds in activated
sludge treatment found that the active fraction of biomass in a mixed system treating
a mixture of organic compounds may be estimated by the fraction of the organic
loading attributable to the individual compound of interest (Magbanua et al.. 1998).
If this is true the active biomass toward the gaseous contaminants may be small since
waste water carbon loading is often on the order of 120 to 200 mg/l (300 to 800
mg/Ld) biological oxygen demand (BOD). The concentration and type of bacteria
that are actively degrading the gas contaminants determines the biodegradation
kinetics and therefore the liquid concentrations of the contaminants. The system
should maintain low dissolved contaminant concentrations to optimise mass transfer
efficiency and prevent discharge in the eft1uent water.
The significant loading of carbon from the contaminated waste water means
that oxygen transfer will generally control the design of the gas delivery system. To
prevent the slowing of aerobic bacterial processes owing to low dissolved oxygen
(DO) concentrations, DO greater than 1 mg/l is generally desired. The relatively high
DO coupled with the low solubility of oxygen means that the mass transfer of
oxygen is inefficient. At inlet gas concentrations of 20% oxygen, eft1uent gas from
activated sludge basins generally contains 13-18% oxygen. Since most volatile
organic contaminants have a much higher affinity for the liquid phase versus gas
phase compared to oxygen (as evident by lower Henry's coefficients). the system is
generally over designed for mass transfer ofthe gas contaminants.
One critical element that should not be overlooked in the design of gas
treatment in activated sludge tanks is the influence of the liquid characteristics on
mass transfer from the gas. For example, in treating waste water it has been observed
that the oxygen mass transfer coefficient (K1a) is generally lower in the waste water
plus biomass suspension (activated sludge) than in clean water. This effect has been
characterised by 'alpha' (a), where:
K, a in wastewater
a (9.1)
KI a in elean water
Activated Sludge 219
Tewari and Bewtra (1982) measured alpha values for oxygen in waste water
of 0.67 to 0.925. A variety of compounds in the waste water could cause this effect
ineluding the biomass itself, surfactants (from soap and biological surfactants), ions,
etc .. Bielefeldt (1996) found that 200 mgll of methanol in tap water resulted in an
oxygen alpha of 0.63 compared to methanol-free tap water. However, the ratio of the
Kla of BTEX (benzene, toluene, ethylbenzene, xylenes) compounds to the Kla of
oxygen was the same with or without methanol. This indicates that the alpha values
for mass transfer of oxygen and BTEX compounds were the same. Roberts el al.
(1984) tested the stripping of five chlorinated organic compounds via bubble aeration
in various types of liquid. Using oxygen transfer as a metric for comparison they
found an alpha of 0.8 for oxygen transfer into filtered secondary effluent. The ratios
of the K1a of the VOCs to the Kla of oxygen were not significantly different in
deionized water and filtered secondary effluent. These relationships are shown
mathematically in Equation 9.2:
Rearranging Equation 9.2 indicates that the VOC u is equal to the oxygen u.
In any case, the mass transfer characteristics of a selected gas sparging device may
differ between clean water tests (as generally reported by manufacturers or measured
in laboratory tests) and full-scale application in systems treating contaminated water.
The characteristics of the liquid in the activated sludge system can also
influence both the Henry's coefficient (H) and the diffusivity in water (Dw) of
oxygen and contaminants. Changes in the Henry's coefficient generally relate to
changes in the solubility of the compounds due to co-solvent effects. The Henry's
coefficient is critical because it reflects the compound's affinity for the air versus
liquid phase. Diffusivity in water controls the resistance to mass transfer from the gas
to liquid.
The characteristics of the liquid in the reactor are important and should be
taken into account during design. Owing to the variability of these conditions and
difficulty quantitatively predicting their effects, bench scale tests may be required
prior to full-scale design.
for compounds with a Henry's coefficient (H) of less than 0.4 (given an oxygen K,a
of 0.24 min-' for a QglA of 100 l/min.m2). Estimating the power required to operate
the gas blower, this shallow reactor depth requires approximately 76% less energy to
operate the blowers than a traditional activated sludge reactor. To achieve a maximal
compact design air diffusers should be located at a somewhat closer spacing with
gre ater coverage of the reactor floor area than is typical for activated sludge reactors
treating waste water. To date, full-scale suspended growth bioreactors designed
explicitly for gas treatment have not been reported in the literature.
treated gas
1-3m
O O o liquid
rising gas O depth
o bubbles o o
o O o
water with nutrients, o
pH buffer, etc. b 'be te r ia I o
,f----- suspeo"sioR
o o
o
o
I contaminated
air diffusion device
I gas
~ _ _ _ _ _ s~ttI~dl:~i0!!la~s i!:e~rn_a<:!!v~e~ sl~d9!l) _ _ _ _ _ _ _ _ j
Most suspended growth gas treatment systems are designed for aerobic
biodegradation of the contaminants with the contaminated gas supplying oxygen to
the bacteria. In these cases, it is possible that oxygen requirements rather than
contaminant removal will control the reactor design. Since the contaminants being
treated in the gas phase are frequently at dilute concentrations, the mass transfer of
the contaminants rather than oxygen may still control the design.
A variety of liquid pumping methods used in bench-scale gas treatment
systems could be applied to full-scale reactors. A mechanical mixer can be used in
addition to the air flow to achieve good mixing of the liquid and suspension of the
bacteria. Desired bacterial nutrients and buffers should be added into the in1et water
to the reactor. To treat organic contaminants, nitrogen and phosphorus should be
added at stoichiometric requirements of about 14 g N and 3 g P per 100 g of C. The
inlet water should also contain sufficient alkalinity to maintain the pH of the system
in a range that is optimal for the bacteria that degrade the contaminants. A
continuous flow ofwater or batch feeding at selected intervals can be used to operate
the system at a selected hydraulic residence time (HRT). This water flow will also
serve to remove metabolic by-products of the bioreactions that might otherwise
accumulate to inhibitory levels. Inhibitory by-product accumulation was noted by
Neal and Loehr (2000) and Bielefeldt (1996) in SGRs treating toluene and BTEX,
respectively.
Another key element in achieving an efficient system is to maintain a high
concentration of biomass in the reactor. This biomass can then rapidly remove the
Activated Sludge 221
concentric·loep
split·cylinder externalloop
3. Process variables
To fully and accurately define the operation of suspended growth gas treatment
reactors, a number of parameters are typically used. They are sometimes slightly
different from those defined for other reactors used for air pollution control and
described in Chapters 3-8. These parameters can be used to estimate reactor
performance and are used in the reactor modelling equations presented in Section 4.
Since different terms are traditionally used by civil engineers for activated sludge
reactor design, environmental and mechanical engineers for gas treatment reactor
design, and chemical engineers for airlift design, a set of parameters has been
selected by the author from these various pools for use in this chapter. Definitions for
the key reactor design and operating parameters and their importance are provided
below, with correJations to terms common to the various literature sources provided.
The reported ranges of selected parameters for the different sub-classes of suspended
growth gas treatment bioreactors are summarised in Table 9.1.
Mean Gas Residence Time, tR = V g/Qg. Mean gas residence time is the
average time that an individual gas bubble is in contact with the liquid in the reactor.
This parameter is frequently not measured but commonly ranges from 1-5 seconds
depending on the bubble size and reactor depth.
Gas Hold-Up, E = V g I (V g + VI). Gas hold-up is equivalent to the gas void
fraction in the reactor which is the volume fraction of the gas phase dispersed in the
total gas-liquid phase. E has a theoretical maximum of 0.74 aud an operational
maximum in the riser of an airlift reactor of 0.3. The gas hold-up in typical activated
sludge tanks aud sparged suspended growth reactors, bubble columns, and the riser
of external loop airlift reactors, concentric internal loop airlifts, aud split cylinder
airlift reactors are approximately 0.005, 0.05-0.2, 0.02-0.2, 0.05-0.2, aud O.OS-O.l3,
respectively (Chisti, 1989).
Empty Bed Retention Time, EBRT = VI/Qg. EBRT is equal to the liquid
volume in the reactor divided by the gas flow rate. Although this parameter is not
truly useful for modelling reactor performance it is easy to calculate and frequently
reported. It also allows a basis of comparison to biofilters where the EBRT is
commonly reported.
Superficial Gas Velocity, Ug = Qg/A. Ug is the volumetric gas flow rate per
unit area of reactor. This is important when there are land or space limitations for a
given reactor. The information can also help to predict the potential for coalesced gas
bubbles versus maintaining discrete fine bubbles of gas in the reactor. Approximate
values ofUg range from 0.001 to 0.2 mls for bubble columns and 0.06 to 0.6 m/s in
the riser of airlift reactors (Chisti, 1989).
224 A.R. Biele{eldt
Mass Loading Rate, MLR = Cgin Qg ! VI. The mass loading rate is equal to the
mass of contaminants entering the reactor per volume of liquid in the reactor per
time. The higher the mass loading ratc that can be treated to the required level, the
smaller the volume of the reactor. This parameter is again useful for comparing
between different types of gas treatment bioreactors.
Specific Loading Rate, SLR = Cgin Qg ! X. Specific loading rate is the mass
loading rate normalised to the concentration of biomass in the reactor liquid or the
mass of contaminant per mass of bacteria per time. If the specific loading rate is too
high the biodegradation capacity of the bacteria in the reactor can be overwhelmed.
This will result in thc contaminant accumulating in the reactor liquid thereby
decreasing mass transfer. In addition, for some organic and inorganic contaminants
high liquid concentrations may be inhibitory to the bacteria. '1'0 prevent accumulation
of the contaminant, the specific loading to a suspended growth bioreactor should be
maintained below the specific degradation rate of the bacteria for the contaminant.
The specific degradation rate of the contaminant varies as a function of temperature,
oxygen concentration, pH, and the Iiquid concentration of the contaminant. The
specific degradation rate is discussed in more detail in Section 4 for modelling.
Overall mass transfer coefficient for the reactor, Kla (units: time- I ). Kla
describes the rate of mass transfer from the gas into the liquid. It is generally
predominated by liquid film resistance to mass transfer (gas phase resistance is
assumed negligible). The Kla includes both the mass transfer resistance (k l) and the
gas:liquid contact area for mass transfer (a). Because it is difficult to measure or
compute the total surface area of the numerous gas bubbles of varying size that are
present in the re actor (a), Kla is measured as a lump parameter. Despite the
importance of Kla for defining the gas:liquid mass transfer characteristics of a
system, it has not been reported for many activated sludge systems or fermenters. Kla
is influenced by the reactor geometry, aeration device, gas flow rate, liquid
turbulence, temperature, and the chemical composition ofthe Iiquid. For example, in
airlift reactors the height of liquid affected the oxygen Kla (Chisti. 1989). In both
bubble columns and airlift reactors, increased solids concentration decreased the
oxygen Kla (Chisti, 1989). The mass transfer coefficient is also frequently correlated
to the power input per liquid volume. More discussion on Kla is given in Section 4.
Table 9.1. Range of aeration and oxygen mass transfer coefficients for different reactors
Reactor Qg/A, Liq depth Temp Oxygen Air addition and References
type (cm/min) (m) (OC) Kla, (min-') mixing
Activated 3-30 4.5-7.6 Env. 0.17-D.38 Ceramic or US EPA, 1989
sludge membrane diffusers Metcalf & Eddy,
at standard flaor 1991
coverage
Sparged 95 0.6-1.22 22-24 1.48-1.8 Ceramic fine Romain, 1996
suspended bubblc diffuser
growth 100% flaor
(SGR) coverage
1.5-16 0.40-D.42 19-26 0.25-D.73 sparge stone Bielefeldt,1996
NR ('.'- stirring) Neal and Loehr,
2000
Bubble 50-1700 1.4-6.0 20-22 O. 18-4.2 non-porous plate Chisti. 1989
column
Airlift 120-1800 1.4-5.2 20-22 0.12-6 non-porous plate Chis ti, 1989
Activated Sludge 225
4. Modelling
Equations describing gas-liquid mass transfer for fine bubble aeration have been
developed based on the two-film theory (Whitman, 1923). In any reactor with a
se1ected aeration device and 1iquid volume, and operated at a given temperature and
gas flow rate, there is a definitive gas-liquid volumetric mass transfer coefficient for
each compound in the system called K,a. According to the two-film theory. in a
system with turbulent mixing, the total resistance to mass transfer across the
interfacial films is the sum of the diffusional resistance due to the liquid film and gas
film. A higher resistance is represented by a smaller mass transfer coefficient (k).
(9.3)
For many compounds, the diffusivity in gas (Da) is much larger than the
diffusivity in liquid (Dw) resulting in less mass transfer resistance in the gas film. In
addition, for compounds with a much greater affinity for the gas phase than the liquid
phase, the H is large. These two factors contribute to the second term in Equation 9.3
being negligible compared to the liquid film resistance. For example, with oxygen,
the gas film resistance is considered negligible and the overall mass transfer rate can
be related simply to the liquid film mass transfer in which the oxygen diffusion rate
affects the transfer rate to the liquid. If liquid film resistance controls the mass
transfer of both a contaminant (such as a volatile organic compound, VOC) and
oxygen, then the K,avoc should be re\ated to the K,ao2 and the ratio of the molecular
diffusivities ofthe compounds in water. This is shown by Equation 9.4,
(9.4)
where Dwvoc is the diffusion coefficient of the contaminant in water (cm 2/s) and
DW02 is the diffusion coefficient of oxygen in water (cm2/s), and n is a constant.
(9.5)
where T = temperature in cc, and e is a coefficient that varies with test conditions,
averaging 1.024.
n = 1 (Bie1efe1dt, 1996). These Kla ratios did not vary significantly at different liquid
depths or gas flow rates that encompassed PIV I from 3 to 46 W/m 3 .
The fundamental differential equation that describes the change in the
contaminant (such as a VOC) concentration in the bubbles of contaminated gas
sparged into the reactor as they rise through the liquid is:
dCg(t) (9.6)
dx
where Cg is the VOC concentration in the gas (mg/l), VI is the liquid volume in the
reactor (m\ Vg is the volume of gas bubbles in the re actor liquid (m\ Klavoc is the
overall mass transfer rate of the VOC in clean water (min·\ a = constant to correct
for mass transfer in activated sludge water versus clean water, CI is the VOC
concentration in the liquid (mg/l), and t is the time the gas bubble has risen in the
column (min).
At t = O, Cg(O) = Cgm, which is the VOC concentration in the influent gas
(mg/l). When t = the total bubble retention time in the re actor, Cg (tR) = CgOll!, which
is the VOC concentration in the effluent gas (mg/l). Although the VOC concentration
in the rising gas bubbles are changing with depth in the reactor, the liquid
concentration in the reactor can be considered constant in a well mixed activated
sludge system at steady state. Under steady state conditions, Equation 9.6 can be
solved for the VOC concentration in the effluent gas, yielding Equation 9.7:
where Qg = gas flow rate (m 3/min), D = the liquid depth in the activated sludge tank
(m), and A = the floor area of the tank (m2 ). This equation is equivalent to equations
used to describe bubble columns by Andrews and Noah (1995; Equation 9.15) and
airlift reactors by Cesario et al. (1995; Equation 9.1).
If biodegradation maintains extremely low contaminant concentrations in the
reactor liquid, the second terrn on the right hand side of Equation 9.7 becomes
negligible; gas treatment efficiency is then controlled by mass transfer and can be
estimated using the first term in Equation 9.7.
(9.8)
228 A.R. Bielefeldt
dS
(9.10)
dt
where Ki is an inhibition parameter for the toxic substrate. If oxygen (or the required
electron acceptor) is limiting, a second term can be added to the Monod expression in
Equation 9.8 to reflect that removal rates become slower when oxygen is limiting
(generaIly below 2 mgll DO).
Since an activated sludge reactor is a continuously stirred tank with SRT
control, the steady state liquid substrate concentration can be described based on
Monod kinetics by rearranging Equation 9.8 (Metcalf & Eddy, 1991):
Ks (1 + b SRT) (9.11 )
CI = [SRT(Yk _ b)] - 1
where Y = the cell yield on the substrate (g biomass/g substrate), b = the biomass
endogenous decay (day"), and SRT = the operational solids retention time of the
reactor (dai'). This allows an estimation of the liquid concentration of the
contaminant under steady state conditions given the biokinetics and operating SRT.
If a group of contaminants is being treated simultaneously, there are two
scenarios that may apply. First, there may be different groups of bacteria within a
mixed culture that degrade various contaminants without direct interaction (such as
an activated sludge system). In this case no changes in biokinetics are needed to
account for treating the mixture of contaminants.
For the case where multiple contaminants present in the gas, such as BTEX,
can be degraded by the same bacteria, competitive inhibition kinetics may be used to
predict the biodegradation rates in the reactor by adding an inhibition (I) term to the
standard Monod equation. 'I' is based on the steady state concentrations of
competing compounds in the reactor Iiquid (mg/l) and the Ks values ofthe competing
compounds (the vaIidity ofthis model was shown in Bielefeldt and Stensel, 1999b).
For two compounds that competitively inhibit one another and only one serves as a
Activated Sludge 229
Ks 1 + b SRT (1 + ~ITCE)
STCE
(9.12)
SRT (kY - b) - 1
Under steady state conditions, the mass transfer rate ofthe contaminant out of
the gas into the liquid must equal the biodegradation rate and washout rate:
(9.13)
Compound Qg/A VOCKla Biokinetics Cgin, eg out, CI, SRT, D, X, (mg/I) DO,
(crnlmin) (min") (mgll) (mgll) (mgll) (d) (m) (mg/I)
Toluene K = 1.0 glg.d 0.1 0.002 0.003 321 12 20 8
H = 0.25 K,=0.18mgll 0.02 0.008 41.3 l.l 30 7
Dw= 1.09 100 0.93 Y = 0.8 g/g 0.02 0.02 14.3 1.15 10 8
b = 0.01 dai' 10 0.2 0.08 4.2 1.1 30 <0.1
10 0.02 0.02 14.3 1.76 65 I
k = 1.0 g/g.d 0.1 0.002 0.008 ** ** ** ** ::....
K, = 0.18 mgll 0.02 0.03 43 4 C)
I 70 1.2
100 0.93 Y = 0.8 g/g 0.02 0.06 1.45 5 ~.
10 7 t:)
b = 0.1 dai' 10 0.2 0.08 6.8 LI 49 <0.1 ~
10 0.02 0.04 22 1.9 91 <0.1 t:l...
100 1.29* k = 1.0 g/g.d 0.1 0.002 0.003 32\ 0.85 29 8 S:2
::::
18.6 0.36 K, = 0.18 mg/l 0.1 0.002 0.003 32\ 0.6 7 8 ~
18.6 0.36 Y = 0.8 g/g la 0.02 0.06 5.3 1.0 8 3 '"
b = 0.01 dai'
0.\ 0.002 0.\ \0.\ 0.16 146 7
0.02 0.1 10.\ 0.10 83 <0.1
Naphtha1ene 100 0.73 k = 0.45 glg.d 0.02 0.2 6.3 0.11 52 <0.1
H = 0.02 K, = 0.25 mgll 10 0.2 0.\ 10.\ 0.10 281 <0.1
Dw= 0.86 Y = 0.85 g/g la 0.2 3.4 0.10 833 <0.1
b = 0.01 dai'
I 0.004 0.1 la 0.15 56 1
10 0.014 0.9 3.6 1.3 22 0.9
* estimated from K1a oxygen ifn = 0.5 in Equation 9.4
** washout condition: cannot achieve such a low substrate concentration; b must be less than 0.03 dai l
tv
'-
"'"
232 A.R. Bielefeldt
4.4 POWER
Since one of the primary operating costs associated with suspended growth
bioreactors is the energy to operate the blower, it is important to estimate the power
requirements ofthe system. From Metcalf & Eddy (1991):
5.10DOURS
Table 9.3. Summary of compounds treated in suspended growth gas treatment bioreactors
References: IOstojic el al., 1992; 2Bowker, 1996; 3Ryckman-Siegwarth el al., 1992; 4Romain,
1996; sCard, 1998; 6Dasu el al., 1993; 7Basu el al., 1996; 8CRC, 1998; 9Vanderberg-Twary el
al., 1997; \OWei el al., 1999; IIRitchie and Hill, 1995; 12Bielefeldt and Stensel, 1999; 13Neal
and Loehr, 2000; 14Landa el al., 1994; 15Bielefeldt, 1996; 16Ensley and Kurisko, 1994;
17Hecht el al., 1995; 18 Zuber et al., 1997; 19Sublette and Sylvester, 1987.
234 A.R. Bielefeldt
Table 9.4. Full-scale waste water treatment facilities treating odorous air in activated sludge
basins.
Diffuser plugging is also a concern but has rarely been reported. Because of
this concern, Ostoj ic et al. (1992) recommends that odorous gases be treated via
coarse bubble diffusers to prevent c10gging or fouling of fine diffusers. However, it
is not apparent that this is necessary. Of the information available 16 plants used
coarse bubble aeration and 14 used fine bubble aeration (note that some plants have
used both, in general switching from coarse to fine when facilities were upgraded).
No problems have been reported more frequently using either diffuser type. It is
important to note that diffuser fouling can also occur in activated sludge tanks
sparged with c1ean air (instead of contaminated air).
It appears that fairly typical blower and sparger maintenance can minimise
any potential problems of treating odour gases. The accumulation of sludgy material
in air pumps has been reported in some cases (Lexington KY, Long Beach CA, Los
Coyote CA, LowelI MA, Ventura CA; Ryckman-Siegwarth and Pincince, 1992). It is
possible that smalI quantities of this material actualIy he1p to protect the blower
materials from corrosion (Bhattarai, 2000).
between inlet concentrations and the detection limits, successful treatment of odour
compounds was achieved in the specifically designed SGR at liquid depths much
shallower (down to 0.6 m) than traditional activated sludge tanks used for full-scale
treatment (4.5 to 7.6 m).
When tests were conducted with unacclimated biomass (35 I of activated
sludge; depth 1.27 m) in the same reactor, concentrations of H2S were reduced from
4 to 5 ppmv to < 0.1 ppmv, but detectable concentrations of amines, ammonia, and
mercaptans were present in the effluent gas, representing 20 to 43%, O to 44%, and
47 to 90% removal, respectively. This indicated that a bioconsortia acclimated for
degradation of odour compounds was critical to achieve good gas treatment
efficiency in the reactor. With the unacclimated biomass, biodegradation, rather than
mass transfer, limited the gas treatment efficiency.
5.2 INORGANICS
The primary use of biologic al gas treatment for inorganic compounds has been
proposed for treating sulphur based contaminants associated with fuels. This includes
both desulphurisation of natural gas (Basu et al., 1996) and treatment of S02 in
combustion off-gases (Dasu et al., 1993). The presence of NO in combustion off-
gases may also be treatable in a suspended growth bioreactor (Dasu et al., 1993).
Treatment of these three inorganics has been studied in lab-scale fermenters. Reactor
operating conditions are summarised in Table 9.5 and the results are discussed in
more detail in the following subsections.
Activated Sludge 237
Cmpd Liquid Qg/A MLR SLR EBRT K,a Inlet Removal Temp
depth, (cmlmin) (mg/ (g/g VS.d) (min) min- I conc, % (DC)
(m) l.h) (t R, s) VOC (mg/I)
(0,2
H2S(1) 0.2 0.3 9.8-20 0.59-1.2 47 NR 7-15 >99 30
(1-2)
H2S(2) 0.15 0.3-1 56-74 NR > 30.8 NR 38 100 30
56-95 > 24' 38 100
NO(3) 0.2 0.6 8 1.5-8.5 50 NR 6.4-6.7 > 96,10030
S02(3) 0.2 0.6 8-33 0.3-0.6 6.8 NR 0.9-2.7 > 95 30
References: (I)Sublette and Sylvester, 1987; (2)Basu el al., 1996; (3)Oasu el al., 1993; '" with
su!phur removal from the \iquid.
Numbers in italics indicate values not directly reported, that were estimated.
NR = not reported.
was achieved at EBRTs of 23.9 min and above; 77% removal was achieved at an
EBRT of 14 min. This study demonstrated successful treatment ofH 2S.
An alternative sulphur-oxidising bacterium, potentially useful for natural gas
desulphurisation, was studied by Sublette and Sylvester (1987) and Dasu el al.
(1993). Thiobacillus denitrificans is a strict autotroph and facultative anaerobe.
Under anaerobic conditions, nitrate will be used as an e1ectron acceptor and reduced
to nitrogen (N 2 gas). If sulphide is limiting, the bacteria will also grow anaerobically
on sulphur compounds, converting S-2 or S03-2 to So or S04-2. Soluble sulphide is
toxic to the bacteria so careful balancing in the reactor must maintain sulphide levels
below the toxicity threshold (~ 150 mgll).
Gas containing 5000 to 10000 ppmv H2S and 50000 ppmv CO 2 in nitrogen
(N2) was added at approximately 30 ml/min via a ring sparger into a fermenter
(Sublette and Sylvester, 1987). The fermenter contained 1.4 l of a T denitrificans
suspension in nutrient media (which initially contained 5000 mg/l KN0 3). Batch
tests (~36 h) were conducted at 30°C with biomass concentrations ranging from 200
to 450 mg protein/l. In tests with an H2S SLR of 3.3 to 4.1 g/g.d, effluent
concentrations were < 0.07 mg/l H2S when the reactor was stirred at 200 rpm (> 99.1
to 99.55% removal). These effluent H2S concentrations dropped below the method
detection limit when the fermenter was stirred at 300 rpm (>99.95-99.96% removal).
In the batch liquid, H2S was converted into S04, biomass growth occurred, and both
NH4+ and nitrate were consumed. The strong growth of biomass in the system
implies that long-term treatment with T denitirificans would be possible if liquid
flow through the system maintained adequate nitrate and ammonia availability.
Somewhat large quantities of nitrate are needed, averaging 1.6 moi N0 3· per moi
H2S. (Sublette and Sylvester, 1987).
Under higher H2S loadings of 4.5 to 8.9 g/g.d, reactor upsets occurred as
evidenced by some H2S conversion to So, sulphide accumulation in the reactor
liquid, and N20 detected in effluent gas. Under these conditions, H2S removal
efficiency dropped to 96% to 87%. Reactor recovery was possible if the cui ture had
been exposed to the high soluble sulphide concentrations for less than 2 to 3 hours.
(Sublette and Sylvester, 1987).
Other bacteria have reportedly been used for treatment of H2S contaminated
gases, but no direct information on these systems could be obtained. Sublette and
Sylvester (1987) cite a study where Thiobacillus lhioparus was used to remove H2S
from gas that was bubbled through the culture (from G. Yu. Ass and B. Sh. Shpiner,
USSR Patent No. 986,469, 1983). Sublette and Sylvester (1987) also cite the use of
mixed cultures of Beggialoa and Thiolhrix to treat H2S gases in a similar manner
(from Nishihara Environmental Sanitation Research Corporation, Japanese Patent
No. 57,170,181,1982).
Aromatic organic compounds are frequently toxic to humans and therefore many are
c1assified as Hazardous Air Pollutants (HAPs) by the U.S. Environmental Protection
Agency. Due to health concems these compounds are regulated for rele ase into the
environment. The removal of a wide variety of aromatic organic compounds has
been studied in lab-scale suspended growth bioreactors. The BTEX compounds,
which are present in gasoline and solvent vapours, have been the most wide1y
studied. The studies achieving successful treatment of aromatic organics are
summarised in Table 9.6.
Some ofthe results shown in Table 9.6 were generated during short-term tests
where the biomass was not allowed to accumulate and the system was not operating
at steady state. The specific loading in these tests was generally high, such that the
contaminants accumulated in the liquid. Using the second term on the right hand side
of Equation 9.7, it was estimated that 83, 28, and 63 percent of the benzene,
ethylbenzene, and o-xylene in the effluent gas was owed to contaminant
accumulation in the reactor liquid, respectively. This indicates that longer tests
aUowing biomass selection and accumulation could achieve significantly improved
removal efficiency for benzene and o-xylene (Bie1efeldt, 1996).
The types of bacteria used to treat the aromatic organic compounds varied. In
general the aromatic organics studied are all readily biodegradable by a wide variety
of aerobic bacteria which mineralise the compounds to carbon dioxide and water. For
the Landa el al. (1994), Ritchie and Hill (1995) and Wei el al. (1995) studies, pure
cultures of Burkholderia cepacia G4 (formerly Pseudomonas cepacia) and
Pseudomonas pUlida strain IlO (ATCC 17484) were used. Although no mention of
changes in the culture over time was made, it seems like1y that long-term operation
under full-scale conditions would not maintain a pure culture in the bioreactor. Using
a defined mixed culture, Kennes el al. (1993) found that most wild type strains
inoculated into a non-sterile fermenter treating gas contaminated with chloroalkanes
and chlorobenzene were washed out after several weeks. Mixed toluene degrading
bacteria were used in the Neal and Loehr (2000) studies. A culture predominated by
a filamentous bacterium (A-l, ATCC No. 55581; but not pure) and grown on phenol
prior to introduction into the gas treatment reactor was used in studies by Bie1efe1dt
(1996) and Bie1efeldt and Stensel (1998).
In two studies the build up of metabolites during BTEX treatment was noted.
Bielefeldt (1996) and Bielefeldt and Stense1 (1998) found that a brown metabolite
formed from long term BTEX gas treatment by a mixed consortium of bacteria in a
sparged suspended growth reactor. The bacteria were enriched from soil from a
manufactured gas plant and maintained in CSTR degrading BTEX for over 1 year
prior to use in the gas treatment reactor. The soluble metabolites were not
specifically identified but were found to accumulate at high loading (> 20 mg
BTEXll.h) and interfere with BTEX biodegradation. Neal and Loehr (2000) observed
Activated Sludge 241
Compound Reactor Q't!A MLR SLR EBRT K,a !nlet Removal Temp.
depth, (eml (mg/l.h) (glg (min) VOC conc., % (0C)
(m) min) VS.d) (tR,S) (0 2) (mg/l)
(min")
Toluene(l) 0.415 2.71 5 0.88 15.4 NR 1.28 99.4 22-25
1.79 14.2 0.98 23.3 5.52 99.9 20-25
1.48 \7.3 1.37 28.2 8.56 98.\ 20-25
2.\2 30.2 1.02 \9.6 9.83 96.9 22-25
Toluene(2) 0.40 3.8 11.6 0.47 10.5 (0.21 ) 2.1 99.4 22-25
6.4 27 0.43 6.7 (0.34) 3.0 98.6
(1.2)
Toluene(3) 0.16- 0.5-1 59.8 3.88 16 1.67 15.95 99 28
0.08 (2.61)
Benz·(4) 0.40 4.0 58.9 4.02 10 0.\3 9.7 96" 20-2\
(1.2) (0.27)
Ethyl- 0.4 8.0 37.2 2.38 5 0.16 3.1 91" 21
benz.*(4) ( 1.2) (0.39)
o-Xylene(4) 0.4 8.0 34.9 1.05 5 0.12 2.9 89" 25-27
(1.2) (0.39)
T_OX(2) 0.4 5.8 21.2 0.37 6.9 (0.31) 1.5/1 98.3 23-25
(1.2)
BT(2) 0.4 6.4 15.6 0.32 6.25 (0.34) 0.8/1 98.8 21-23
( 1.2)
BTE(21 0.4 5.2 \6.0 0.32 7.7 (0.28) 0.7/0.8. 98.2 22-24
( 1.2) /0.7
BTEX(21 0.4 4.6 \4.9 0.27 8.7 (0.25) 0.6 ea. 98.2 22-24
( 1.2}
Phenol(51 0.6-0.7 4-32 1.8- 1.3 " 3-22 r 0.65- > 99.7 20-25
r 16.2 (0.83) 0.85
p-Cresol(6) 1.5 r 21 r 1.03- 1.2 * 7r 1.2 0.43 > 99.5 30
2.4 (5) (1.66)
References: (I~eal and Loehr, 2000; (2)Bielefeldt and Stensel, 1998; (3)Landa el al., 1994;
Bielefeldt, 1996; (5)Ritchie and HiII, 1995; (61 Wei el al., 1999; r = riser of airIift; /\ dry
(4l
weight; NR = data not reported; itai ies = values not directly reported that were estimated;
'short term tests (therefore, specific loading rate likely higher than would occur under
steady-state conditions).
242 A.R. Bielefeldt
in a biofilter column packed with compost aud perlite. At mass loadings of 3.9 to
28.1 mgll.h, 96.8 to 99.7% ofthe toluene was removed. The inlet air was humidified
to maintain moisture content in the reactor, but drying aud cracking of the bottom
layer of the reactor was visible on Day 32 in the high loading experiment, which
resulted in a 20% drop in toluene removal efficiency. The treatment performauce
achieved in the biofilter was comparable to the suspended growth system except that
the biofilter was loaded with much higher gas flow rates (1100-2340 ml/min) aud
much lower inlet concentrations (0.09-0.8 mgll) to give the same mass loading as the
suspended growth system.
Compounds Reactor Liquid Qg/A MLR SLR EBRT Kla Inlet Removal Temp. References
type depth, (cm/min) (mg/l.h) (g/gVS.d) (min) (min· I ) concentration (%) (0C)
(m) (t R , s) VOC (mg/l)
(0 2 )
TCE F 0.16- 0.5-1 0.92 0.06 16 1.7 0.24 90 28
+ toluene 0.08 55.2 3.53 (2.6) 14.7 99
TCE A 0.30 •• 2.0 6.86 1.5 35 NR 4.0 94 20-25 2 ;,.,
+ phenolliquid 0.51 0.11 35 0.3 97 ~
~.
TCE • B 0.4 4.7 0.5-8.2 0.01--D.16 8.5 0.09 0.07-1.2 77-82 22-24 3 I:l
(1.2) (0.2) ~
I:l..
TCE B 1.5 25 0.7-2.7 0.01--D.05 6 0.13 0.07--D.27 75-80 25 4 ~
+ phenolliquid :::
TCE B 1.5 144 8 0.15 1.04 0.55 0.14 50 25 4
~
+ phenolliquid '"
TCE A 1.5 48-168 15-19 0.25--D.57 1·3 0.18-0.64 0.31-1 50 25 4
+ phenol liquid
DCM A-S 0.83 305 441 NR 0.27r NR 2 85 30 5
A = airlift; A-S = airlift with sand; B = bubble column; F = fermenter;
References: lLanda et al., 1994; 2Ensley and Kurisko, 1994; 3Bielefeldt 1996; 4 Hecht el al., 1995; 5Z uber el al., 1997.
r = riser basis; NR = Not reported; italics = value not directly reported, so estimated;
*short-term test with endogenous toluene-degrading bacteria;
*. reported reactor dimensiol1s nut consistent - 3.5 L Ţ 30 cm depth and 8 cm diameter.
N
....
Uv
244 A.R. Bielefeldl
contaminated rags) were treated via gas recirculation until complete destruction was
achieved.
Zuber el al. (1997) used the results of three years of bench-scale treatment of
DCM in a 3-phase airlift bioreactor (sand:water:air) to estimate scale-up to a full-
scale treatment system. Owing to the presence of the sand the system contained both
suspended biomass and attached biomass. These results are discussed in more detail
in Section 7.1.
compare a bubble column to a concentric loop airlift reactoL Under high TCE
loading conditions where 50% removal was achieved, the airlift system could operate
at a higher MLR and SLR than the bubble column (see Table 9.7). In general, the
treatment efficiency declined with increasing loading (from higher TCE inlet
concentrations and/or higher gas flow rates). The biomass concentrations in the
reactor were high, ranging from 900 to 1650 mg dry weightll.
Bielefeldt (1996) attempted co-degradation of TCE and toluene from
contaminated gas in a 2 1 bubble column containing a filamentous bacterial culture,
but poor treatment efficiency of TCE and toluene were achieved, probably owing to
competitive inhibition effects. Subsequent tests used endogenous cells that were pre-
induced by growth on toluene, achieving 77-82% TCE removal. For long term
operation, this system would require two reactors to continuously treat TCE
contaminated air. While one reactor was treating TCE, the other reactor would be fed
the appropriate co-substrate (in this case, toluene). Then the reactors would switch.
This would have the advantage that co-substrate would not be present during TCE
degradation to compete. In addition, during co-substrate feeding the desired amount
of biomass in the system could easily be controlled without worrying that the
competition would decrease the TCE removal efficiency. Previous studies with the
filamentous culture showed that endogenous TCE degradation could be maintained
over 24 hours after growth on phenol (Bielefeldt et al., 1995). Therefore, the
proposed treatment strategy shows promise for suspended biological reactors treating
TCE contaminated gas on alternating cycles with substrate feeding.
(0.40 mg/l inlet), TCE removal averaged 62% over 25 days; however, TCE removal
was decreasing over time probably owing to toxicity. In a final experiment at a TCE
loading rate of 1.34 mgll.h (0.72 mgll inlet), the removal rate averaged 21% and
remained fairly constant over 25 days of operation. These results are less optimal
than gas treatment of TCE using toluene or phenol as co-substrates.
Dichloromethane (DCM) is somewhat easier to treat since it can be degraded
as a bacterial growth substrate. Ergas et al. (1994) achieved greater than 98%
removal ofDCM in a 211 compost biofilter loaded at 0.57 to 9.5 mg/l.h (inlet 0.01 to
0.19 mg/l). Diks and Ottengraf(l99l) achieved greater than 90% removal ofDCM at
mass loadings less than 50 mg/l.h (inlet 1 mg/l) in a 377 1 lab-scale trickling filter
packed with ceramic saddles and seeded with Hyphomicrobium GJ21. The results
from the attached growth systems cannot be directly compared to the results reported
in SGRs due to the significantly different test conditions.
Wei et al. (1999) investigated the treatment of ethanol contaminated gas in a bench-
scale extemal-loop airlift reactor. The 12 1 reactor was inoculated with Acetobacter
aceti (ATCC 15973) and sparged via a spinning flat disc (giving an oxygen K,a of
approximately 1.67 min"). Ethanol is not fully mineralised by A. aceti with acetic
acid a major by-product. Therefore, growth on ethanol was slow (Y = 0.064). In a
short-term test (80 h), an inlet concentration of 70 mg/l ethanol (mass loading 220
mg/l.h) was treated to > 99% removal from 0.62 l/min gas flow by 800-1700 mg/l
biomass. Ethanol concentrations in the liquid ranged from 150 to 50 mg/l but no
breakthrough of ethanol occurred owing to its high affinity for the liquid phase. It
was predicted that at steady-state conditions with a liquid retention time of 4.2 days
that the steady state biomass in the reactor would be approximately 1500 mg/l.
Vanderberg-Twary et al. (1997) treated contaminated gases from a waste
barrel using a gas loop that was passed through a bubble column bioreactor. The gas
contained methanol, 2-propanol, aud dichloromethane, representing paint stripping
wastes; concentrations were not reported. Biomass concentrations of 75 to 270 mg/l
were able to de grade contaminants from the gas but insufficient data were reported to
determine the mass loading or specific loading to the reactor during the experiments.
The costs for an activated sludge gas treatment system will include both capital and
operating (power, aeration maintenance) costs. Table 9.8 lists the primary costs to
build and operate a suspended growth gas treatment bioreactor. The main costs to
construct a new suspended growth gas treatment basin will be: the basin, the air
diffuser system including piping and diffuser heads, airflow and pressure monitoring
equipment, an air blower, blower controls, liquid feed (and waste) pump, and
biomass separation basin aud retum pump (if needed). Optimal design for gas
treatment resulting in more shallow tanks thau are common for municipal waste
water activated sludge tanks will save money on the bas in and blower (owing to less
head needed). If an existing activated sludge system is present for waste water
treatment little additional capital costs may be required.
In addition to the initial expenditures, operating the system will require
energy, periodic labour for maintenance, and materials. The primary operating cost
Activated Siudge 247
Table 9.8. Costs associated with suspended growth gas treatment bioreactors
for the activated sludge system is generally the power for the blower. This power
requirement is a function of the pressure at which the gas must be injected into the
reactor. The pressure needed is significantly higher than for the other types of gas
treatment systems because it must overcome the head of water (water depth in the
tank) and headloss in the aerator. For example, the headloss across biofilters has been
reported to range from 0.003 to 0.17 m of water head per m of bed depth (Govind et
al., 1993; Kiared et al., 1997; Torres et al., 1997). Equation 9.16 can be used to
estimate the power requirements for aeration (Metcalf & Eddy, 1991). Given nearly
equal head loss across the aerators, regardless of the tank depth, a general
relationship between tank depth (giving the water head of the air to overcome) and
the power required can be generated. Assuming an air flow rate of 100 m3/min (at
standard temperature and pressure) at 0.5 m and 5 m liquid depths, the blower power
required is approximately 10.4 and 91.7 kW, respectively. This indicates an energy
savings of about 88% in the shallow reactor. The nutrients and buffer chemi cais
added to support biogrowth (such as nitrogen, phosphorus) may also be a significant
operating cost. Maintenance required for the suspended growth system will include
periodic cleaning andlor replacing diffusers, and routine maintenance for the
blowers, liquid pumps, and instrumentation.
Zuber el al. (1997) estimated that a basic investment cost of $174300 would
be needed to construct an airlift re actor with sand media to treat 100 m3/h of air
containing 2 mg/l dichloromethane to 99.5% removal. Additional operating costs for
energy, chemicals, water, and personnel time averaged to $79720/yr. Bowker (1996)
estimated the cost to treat 3738 m 3/h of odour gases, including 0.18 mg/l H2 S, in a
dedicated SGR at $230000 capital and $95000/yr operation and maintenance.
However, the analysis assumed that a 4.27 m deep tank would be needed (a
traditional tank depth for a waste water treatment activated sludge basin), which is
significantly higher than the depth that would actually be needed. The model
248 A.R. Biele{eldt
indicates that a significantly lower depth can be used (about 1 m), saving both capital
costs (smaller basin, smaller blower) and operating costs (energy for blower).
For specific cost estimates for blowers, fine bubble diffusers, and
maintenance costs for activated sludge aeration, the US EP A Design Manual "Fine
Pore Aeration Systems" (1989) offers a good, though old, summary of data. Using
this information the cost of treating gases in an optimally designed SGR has been
estimated. Costs are adjusted to 1996 values using ENR cost indexes in order to
compare to the Zuber and Bowker values. The test case was treating 2 mg/l toluene
in 100 m3/h contaminated gas to 99.5% removal. Using the modelling method
described in Section 4 it was determined that a tank with 0.75 m liquid depth and 9
m2 area could be used (operating at a Qg/A of 18.6 cm/min). This system operated at
a 31 d SRT to give a toluene concentration in the liquid of 0.01 mg/l, biomass
concentration of 12 mgll, and adequate oxygen was available ( > 2 mg/l DO if the
inlet air contains 20% oxygen). The long SRT and small volume ofthe tank require
only a very small liquid pump, perhaps operated once every three days to feed
nutrients to the reactor and waste liquid contents. Capital costs for purchase,
construction, and installation of the tank, diffusers, blower, liquid pump, nutrient
feed tank, electrical, and plumbing would total $7000 to $9000. Energy costs for the
blower, liquid pump, chemical costs, and labour cost for maintenance would total
about $14000/yr. To treat 4000 m 3/h ofthe same gas and treatment efficiency, a 360
m2 x 0.75 m deep tank would be needed, at a capital cost of about $190000 to
$250000 and yearly cost of $90000 (realising economy of scale). These costs
compare very favourably with the previous estimates of Zuber et al. (1997) for the
airlift reactor and are similar to those from Bowker (1996) for odour treatment.
7. Variations
Solid carriers such as activated carbon, plastic media, or sand can be added into the
sparged system. Depending on the amount of solid carrier added, the re actor may end
up more similar to a fluidised bed reactor than a suspended growth system. A
significant amount of the total biomass in the reactor may be attached to the solid
carriers in a biofilm rather than being suspended in the liquid. This should result in a
longer mean retention time of bacteria in the system since they will not be washed
out with the liquid. The addition of activated carbon into the SGR may enhance
reactor operational stability and performance due to its sorption capacity. Ye et al.
(1994) modelled the addition of activated carbon into the riser of a concentric-loop
airlift reactor. In the 5.5 m deep liquid, the model predicted > 90% removal of
benzene or toluene, and greater than 97% DCM removal. No information on the
mass transfer characteristics of the airlift reactor and activated carbon concentration
were provided, and the modei was not experimentally validated. Zuber et al. (1997)
studied treatment of DCM contaminated gas in a concentric loop airlift reactor
Activated Sludge 249
Cesario et al. (1997) proposed the use of a co-solvent to improve mass transfer into
water. The water-immiscible solvent is dispersed in the liquid and the contaminant of
interest (and/or oxygen) has a higher affinity for the solvent than water. The solvent
FC40 was chosen to study toluene removal (conc. gas/conc. solvent = 0.012
compared to H of 0.21 for toluene). FC40 is a perfluorocarbon that is non-
biodegradable, non-toxic, and has a low vapour pressure (so it will not be lost to
volatilisation). The FC40 was maintained dispersed by mechanical mixing at 800
rpm. The K1a oftoluene (0.017 S-I) was not influenced by volumetric concentrations
of 0-10% FC40. Similarly, the oxygen K1a was also insensitive to FC40 conc (0.017
S-I). In the presence of 10% of FC40, the toluene mass transfer was enhanced by a
factor of 1.1 (mass transfer with versus without solvent) and oxygen by a factor of 2.
This indicated a negligible benefit for contaminant treatment unless oxygen supply
controlled the reactor design. However, different co-solvents might prove more
successfu!.
8. Conclusions
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PART 2. APPLICA TIONS
CHAPTER 10 BIOFILTRATION OF WASTE GASES FROM
A DAIRY INDUSTRY
Christian KENNES
1. Background
Biological waste gas treatment in above ground conventional biofilters using natural
filter beds is a simple and efficient technology (Chapter 3). It is suitable for the
treatment of polluted air originating in production plants and waste water treatment
plants from food and drinking industries (Passant et al.. 1992). The technology has
recently been app1ied by Casals Cardona Ind. for the treatment of waste gases
released from a waste water treatment plant and containing mainly su1phur
compounds, ammonia and some VOCs.
2. Technology selection
Preliminary studies showed that the mean waste gas flow rate reached 4000 m 3/h and
was mainly composed of a mixture of low concentration organic and inorganic
volatile pollutants (Table 10.1) released at ambient temperature. The VOC mixture
was mainly composed of lactic acid and low concentrations of several non-identified
volatile fatty acids.
The main reasons for the biofilter vendor (Casals Cardona Ind.) and for
members of the dairy industry to select a biological process for solving the air
pollution problem were the low investment and operation costs compared to other
technologies. high efficiency and minimal supervision and monitoring requirements.
Biodegradability of the pollutants is a prerequisite for applying biofiltration.
Several studies have shown that the compounds listed in Table 10.1 can relatively
easily and completely be mineralised under aerobic conditions (Weckhuysen et al.,
1994, Smet and Van Langenhove, 1998). The above mentioned gas flow rates and
temperature are also suitable for biofiltration. A conventional biofilter was selected
257
C. Kelllles and M. C. Veiga (eds.). Bioreactors for Waste Gas Treatment. 257-260.
© 2001 Kluwer Academic Publishers.
258 C. Kennes
as it represents the simplest and cheapest design and because ofthe recent experience
of Casals Cardona Ind. in operating such systems. Although biodegradation of
sulphur compounds might lead to pH drop, many of the microorganisms degrading
such compounds are known to be quite resistant to acidic conditions, although VOC
degraders might be more sensitive. The presence of ammonia in the waste gas might
also partly buffer pH fluctuations in the presence of metabolites formed during
biodegradation of sulphur compounds (Chapter 3) (Kennes and Thalasso, 1998). It is
also worth observing the quite low concentration of pollutants representing in fact
conditions typical of odour problems to which biofiltration technology was applied
originally. It can easily be calculated that mass loading rates of only a few g/m 3 .h
were applied. Such low concentrations will also contribute to maintain limited pH
variations. An advantage of using a natural carrier is that it can be used as organic
fertiliser when it gets exhausted and once it needs to be replaced for maintaining
proper operation ofthe bioreactor.
3. Biofilter design
A 4 kW centrifugal fan made out of non-corrosive material was used for polluted air
ducting from the emission source to the treatment system at a flow rate of 4000 m 3/h,
trying as far as possible to avoid mixing c1ean air with the polluted air stream which
would otherwise generate higher flow rates and increased energy costs. The parts in
contact with the fluid were made of a biphenolic resin/fibre glass mixture.
3.1 PRE-TREATMENT
3.2 BIOFILTER
volume of water added daily to the system was approximate1y 200 litres, value that
could either be increased or decreased depending on weather conditions. The bottom
and walls of the biofilter were recovered with a impermeable layer made of
thermoplastic materials.
The biofilter has been operating for approximately two years so far. It was not
inoculated and the start-up period lasted about one month. Although inoculation with
speciali sed cultures has proven to be sometimes necessary when dealing with methyl
sulphide pollution (Smet el al., 1996), this appeared not to be a prerequisite in the
present case, although such a procedure would have been interesting if a shorter
start-up stage was required. Although sampling effluents of such open biofilters is
difficult, monitoring data allowed showing that the start-up period was characterised
by overall removal efficiencies of about 40-60%. Sampling was undertaken by
placing a hood provided of a stack above the biofilter bed. After the first month
operation, removal efficiencies could be maintained above 60% most often reaching
above 99% removal, and eliminating complaints conceming odorous emissions.
After almost two years operation, pressure drop was still minimal. Previous
experience of Casals Cardona Ind. with such filter beds has shown that after two to
three years continuous operation, the addition of 30% fresh carrier material would be
required. The total lifetime of the carrier under the present running conditions is
expected to reach five years. After such a period, complete renewal of the filter bed
is necessary as a result of one or several ofthe following potential problems (Chapter
3):
• Bed compaction;
• Excess dead biomass;
• Exhaustion of relevant nutrients of the filter bed;
• Presence of high salt concentrations;
• Channelling effects;
• Excessive accumulation of dust particles.
The old filter bed is advantageously used as fertiliser. Experience has shown that
covering the filter-bed with a special grass layer may be useful for improving and
maintaining optimal moisture conditions and to avoid unwanted growth of weed or
the presence of large roots eventually altering homogeneity and composition of the
filter-bed. Such a procedure also improves the general aspect ofthe biofilter.
References
Kennes, C. and Thalasso, F. 1998. Waste gas biotreatment technology. l. Chem. Technol. Biotechnol.
72: 303-319.
Passant, N.R., Richardson, S.J., Swannell, R.P.J., Woodfield, M., van der Lugt, l.P., Wolsink, l.H.,
Hesselink, P.G.M., Hecht, V., Brebbermann, D. and Bischoff, H. Biodegradability of the volatile
organic compound (VOC) emissions from the food, drink and metal degreasing industries. In:
Biotechniques for Air Pollution Abatement and Odour Control Policies. Dragt A.J. and van Ham J.
(eds.). Eisevier, Amsterdam, The Netherlands, 1992, pp. 315-320.
Smet, E., Chassaya, G., Van Langenhove, H. and Verstraete, W. 1996. The effect ofinoculation and
the type of carrier material used on the biofiltration of methyl sulphides. Appl. Microbiol. Biotechnol.
45: 293-298.
Smet, E. and Van Langenhove, H. 1998. Abatement of volatile organic sul fur compounds in odorous
emissions from the bio-industry. Biodegradation. 9: 273-284.
Weckhuysen, B., Vriens, L. and Verachtert, H. 1994. Biotreatment of ammonia- and butanal-
containing waste gases. Appl. Microbiol. Biotechnol. 42: 147-152.
CHAPTER 11 TREATMENT OF HIGH VOC LEVELS IN A CLOSED
BIOFILTER
1. Introduction
Traditionally, biofilters have been used to solve odour problems throughout Europe
and more recently in North America (Leson and Winer, 1991; van Groenestijn and
Hesselink, 1993; Kennes and Thalasso. 1998). Although just as important as the
odour industry, less attention has been paid to biofilters treating volatile organic
compounds (VOC) in the chemical, pharmaceutical, printing and automotive
industries. Poorly designed biofilters have caused a great deal of negative publicity.
Consequently, biofilters in the USA and to a lesser extent in Europe are typically not
considered a reliable and cost efficient solution to VOC emission problems. In
Europe however, partly because of regional strict emission regulations, biofilters
have established themselves as cost effective and reliable VOC abatement solutions
in some industries (Chapter 1). A number of companies have built several full scale
biofilter installations in various different fields including the food, food flavouring
and fragrance, municipal, pharmaceutical and chemi cal industry.
A company in the Netherlands which produces industrial separation
membranes was contracted by the Dutch government to solve their methanol and
trichloroethene (TCE) emis sion problem. Their day time emis sion Ievels were 1800
mg/m 3 ofmethanol and 200 mg/m 3 ofTCE, while a maximum of 100 mg/m 3 ofTCE
was allowed as well as a total VOC maximum of 150 mg/m 3 . Therefore the methanol
concentration had to be decreased to a maximum of 50 mg/m 3 . The TCE levels were
to be decreascd to 100 mg/m3 by alteration of the production process and a
previously installed activated carbon system.
Typically it is assumed that biofiltration is not technically or economically
feasible when treating high levels ofVOC is required. The most common choices for
treating these streams are thermal and catalytic oxidation and adsorption. However,
if an accurate description of the off-gas is obtained a biofilter can be properly sized.
In addition, experience must play a large role in overcoming the practical hurdles in
designing for highly concentrated off-gases. If a biofilter has the proper residence
time, proper moisture addition system and nearly continuous loading, biofiltration
can achieve high removal efficiencies (gre ater than 90%) for methanol in a very cost
effective manner.
2. Technology selection
800000
700000
600000
~
'"
lfJ 500000
2- 400000
t1o 300000
u
''"O
1-<
200000
100000
o
o 3 4
Years of operation
3. Biofilter design
4. Biofilter performance
Soon after start-up of the biofilter system, it was dear that the installation did not
perform as specified. Fourier Transform Infrared Spectrometry (FTIR) analysis ofthe
process gas is shown in Figure 11.3, and indicates an average inlet loading of 2500
mg/m3 and peaks of 3000 mg/m3 . The peak durations were too short for the
microorganisms to adapt, so peaks left the system virtually untreated. Under the
above conditions, the outlet concentration fluctuated between 300 and 500 mg/m3
(approximately an overall removal efficiency of 85%) much more than allowed by
the regulatory body. Measurements also showed that inlet concentrations of TCE
were not reduced during passage of the filter medium. Even on a longer timescale
the inlet and outlet concentrations were the same, indicating that no buffering within
the biological system occurred. The assumption that TCE would have no effect on
the biology was confirmed by the fact that the biofilter performed within the design
limits, taking the desiccation the filter medium and the spiked loading into account.
A detailed investigation of the system revealed that it was not possible to
remove the higher leve1s of methanol with the amount of medium in the system.
Even if the system was fully operating according to the design parameters the
capacity of the system was not sufficient. In addition, owing to the high inlet
concentrations high levels of heat were formed during oxidation resulting in
desiccation of the filter material. Specifically, when heat is generated from bio-
oxidation, moisture is transferred from the filter medium to the air stream. Normally
the automatic moisture addition system would compensate for the moisture lost
through evaporation. However, the pressure of the water in the piping system feeding
the overhead spray nozzles was less than design pressure. This resulted in a
deficiency in the coverage zone of the nozzles, therefore the moisture of the medium
could not be adequate1y maintained. At lower inlet concentrations of polluting
compounds these problems do not result in a critical situation. In this particular case
the rapid desiccation and the limited nozzle coverage created dry areas in the filter
bed (as shown in Figure 11.4). Dry filter material has a lower pressure drop than wet
filter material, so the inlet air tended to flow trough dry filter material. As a result,
not the whole volume of the filter material is active in the degradation of the
methanol. This does also mean that more methanol, and therefore more substrate for
heat production, is preferentially going through the dry areas. A low moisture content
Case study - Closed biofilter 265
3500 , - - - - - - - - - - - - - - - - - - - - - . ,
~3000
~2500
~ 2000 - - Maximum inlet
o
~ 1500 ....... Maximum Qutlet
'E
l'.l1000
1:
O
o 500
W
C O~~~~~~~~~~~~====~--~
o 2 4 6 8 10
Time (days)
has a negative influence on mass transfer from the air to the biofilm, as well as an
inhibiting effect on the activity of the microorganisms. Escape from this vicious
circle is not possible in this normally self-regulating system and appropriate measures
are required to correct the situation and to prevent the eventual failure of the biofilter.
Humiclffieatlon~
$Y$tem
. . -'~Filter meclium
The third problem was the low water pressure causing inadequate water
coverage from the overhead nozzles in the bio-oxidation chamber. Since the water
pressure could not be increased, additional nozzles were installed and the nozzle
layout was improved. The nozzles were rearranged to give a more even distribution
of water of the filter surface. The automatic spraying system was now capable of
humidifying the whole of the filter bed, providing the optimal conditions for the
microorganisms. The even distribution of water also allowed an even distribution of
the airflow through the filter bed, resulting in optimal biological activity throughout
the entire filter medium. Furthermore the even distribution of water created an
increased total specific surface area by improving the exchange surface between
water and air. This allowed the biofilter to take up more methanol out ofthe airflow.
S. Conclusions
After corrective measures were taken, additional off-gas sampling was performed
throughout the system. The results of this sampling are shown in Figure 11.5.
Sampling confirmed the high inlet loading and the day time peak loadings of
methanol. In addition, it was confirmed that the packed bed humidification system
allowed the peaks to be dampened. The more even distribution of water over the
filter surface, resulting in a better use of the total filter medium, led to an improved
performance of the first biofilter vessel. Although the performance was not good
enough to comply with govemmental regulations, the outlet concentrations of 100 -
Case study - Closed biofiller 267
3500
~ 3000
C,
§. 2500
CI)
c::
- - - Maximum inle/
:8 2000
....... Maximum oullel
~
'E<Il 1500 - . - . - 'n'el Me/hano' afler humidifier
(.l
c::
o 1000
a;"
:s 500
Ou!l~t m~!/lanol
o
o 2 4 6 8 10
Time (days)
150 mg/m 3 carne near the required value of 50 mg/m 3 , Finally, it was obvious that by
adding the additional bio-oxidation vessel complete removal of methanol could be
achieved.
Detailed models do exist to determine the volume of medium required for
applications and to predict biofilter performance. However, biofilter performance is
extremely dependent on this sizing tool. If adequate data of off-gas composition do
not exist, it is highly recommended that VOC specification and quantitication
sampling is performed prior ta design. In addition, experience must always be
combined with modelling results when sizing biotilters. Understanding the effects of
heat generated from bio-oxidation, peak loading effects, the importance of
humidification and an even water distribution and other complications can only be
accounted for through empirical data. The present case study is an example of how
combining experience with proven design too1s can provide reliab1e remova1 of high
levels of methanol, a common VOC.
References
Kennes, C. and Thalasso, F. 1998. Waste gas biotreatment technology. J. Chem. Technol. Biotechnol.
72: 303-319.
Leson, G. and Winer, A.M. 1991. Biofiltration: an innovative air pollution control technology. For
VOC emissions. J. Air Waste Manage. Assoc. 41: 1045-1054.
Van Groenestijn, J.W. and Hesselink, P.G.M. 1993. Biotechniques for air poIIution control.
Biodegradation. 4: 283-301.
CHAPTER 12 NEW BIOREACTOR SYSTEM FOR TREATING
SULPHUR- OR NITROGEN- COMPOUNDS
N.J.R. KRAAKMAN
1. Introduction
high water solubilities (Chapter 3). However, conventional biofilters present some
limitations in treating polluted air streams that contain:
Below we will describe a bioreactor system capable oftreating air streams containing
mixtures of compounds like hydrogen sulphide, organic sulphur compounds,
ammonia and organic nitrogen compounds.
• For municipal waste water treatment plants and lift stations the ZEROCHEM
unit has been deve1oped.
Air streams emitted from municipal waste water treatment plants and lift
stations in sewer lines contain odorous gases. The volume of the stream is often
small (mostly up to 2000 m 3/h) and its composition is relatively constant. High
removals of odours, among which hydrogen sulphide, are required in these
situations. The bioreactor should be able to be operated either with or without a fan.
When functioning without a fan the air comes out a dwell only when waste water
enters the dwell. Low pressure drop over the bioreactor is therefore required. Low
maintenance and simplicity of operation are important factors for such application.
• For the Viscose industry the V-SPRING bioreactor has been deve1oped.
Air streams that contain H2S in combination with CS 2 are emitted by Viscose
industries. The volume ofthe streams is re1ative1y large (more than 50000 m 3/h) and
CS2 emissions forrn the driving force to treat them. The emissions of CS2 are
regulated in many countries and conventional air treatment techniques are often not
272 N..J. R. Kraakman
Figure 12.1. A PURSPRING bioreactor treating off-gases from an oii seed extraction plant.
cost-effective. It is important that the air is treated at any time and special
requirements for the bioreactor are necessary because of the risk of explosion linked
to the presence of CS2. The process control is much more complicated and special
training of the operators is required. The degradation of the compounds in
bioreactors is performed by special\y cultivated microorganisms and the degradation
process is control\ed by the salt content of the process water. The pH of the water is
extremely low. In some applications it is desirable that the effluent water coming
from the bioreactor can be reu sed in the production process in the plant.
4. Operating strategies
4. 1 INTRODUCTION
Pol\uted air streams nearly always contain a mixture of very different compounds.
Each application is different and the new bioreactor provides the required flexibility
needed to treat such pol\uted air streams. Examples of different operating strategies
that can be used are mentioned below.
Case study - New bioreactor 273
Figure 12.2. A PURSPRlNG bioreactor treating off-gases from an anaerobic waste water
treatment plant of a brewery.
Polluted air streams often contain a mixture of different compounds with different
chemical properties. These compounds differ from each other in their ability to be
biodegraded and their solubility in water. The compounds need to be transported to
the biofilm and degraded in it. To degrade aII these compounds a specialised mixture
of microorganisms is required. But not aII these microorganisms will present optimal
activity under the same process conditions. Microorganisms differ in their ability to
form a good biomass structure, in their growth rate, in their biodegradation capacity
as weB as optimal pH and nutrient conditions. Besides microorganisms differ from
each other with respect to their capacity to obtain their energy and nutrient sources.
As a result of the presence of different compounds in the air stream different
microorganisms are necessary and therefore different environmental conditions are
required.
One example in which different environmental conditions are preferred is
when a consortium of autotrophic and heterotrophic organisms represents the best
combination to treat an air stream containing a mixture of compounds. Many odorous
274 N.JR. Kraakman
air streams often contain a mixture of compounds that can best be treated by a
combination of autotrophic and heterotrophic organisms. The most optimal way to
treat such polluted air stream is by dividing the bioreactor into different levels
allowing optimal activity of different organisms under different environmental
conditions. Autotrophic organisms can biodegrade H2 S whilc hcterotrophic
organisms will remove odorous compounds separately.
Autotrophic organisms use carbon dioxide as carbon source in the air stream.
In a biofiltration system treating odour compounds these autotrophic organisms often
get the cellular energy for growth and respiration from thc oxidation of H2 S (often by
growing first Thiobacillus spp.). These aulotrophic organisms grow relatively slowly
and show high uptake rates even when sulphuric acid is present at such a
concentration that the pH becomes rather acidic. Heterotrophic organisms use
organic compounds (VOC) to obtain their cell carbon. Their growth rate is often
higher than for autotrophic organisms but they often require near neutral pH
environments.
In the bioreactor autotrophic organisms degrading HzS and heterotrophic
organisms degrading organic compounds are separated in different layers of media.
Because of the low Henry's constant of HzS compared to most other organic
compounds it is most common to degrade HzS in the first layer of thc bioreactor
while the organic compounds can be removed in the second layer. Removal of HzS in
the first layer prevents acidification of the media in the second layer and provides
optimal conditions for growth and survival of the heterotrophic organisms. So by
using different layers with different microorganisms a broader range of compounds
can be biodegraded.
4.3 TRRTGATION
Water can be added on top of each layer of media separately. Not only the amount of
water but also the frequency of irrigation can be regulated separately for each layer.
Water can also be added either continuously or discontinuously to a layer; in such a
way that the thickness of the water boundary can be regulated on the biofilm layer.
The water boundary is necessary for an efficient mass transfer and substrate
utilisation. Too much water leads to less void volume in the media, which is negative
for the removal of poorly soluble compounds. Compounds that are poorly soluble in
water need a long retention time in the media in order to reach efficient mass
transfer. Depending on the differences in compound solubilitics and mass transfer,
the irrigation program per layer must be adapted to each specific situation.
Manipulating the irrigation method per layer can increase the flexibility and air
purification efficiency.
Some additional considerations regarding operating strategy arc mentioned
hereafter. The process water in the bioreactor can either be recirculated over the
different layers or it can be added to one layer and then simply removed from the
bioreactor. When low pollutant concentrations are required in the out1et air stream of
the bioreactor it is better not to recirculate the water over the upper layer. Cleaned air
can otherwise come into contact with a concentrated water phase leading to stripping
of certain compounds from the water phase to the c1eaned air. On the other hand
recirculation can be interesting in some other situations. Microorganisms may get
slowly washed out from the media or they may be partly removed when
environmental conditions are not favourable for some of them in the biofilm.
Case study - New bioreactor 275
The operating strategy can be changed by modifying media composition. In the new
bioreactor an inorganic medium is used. For different situations a different medium
composition is considered reaching either a more open or a less open medium
structure.
By changing media composition the surface area and the void volume can be
made different for each layer. A high surface area is necessary for a proper mass
transfer of the compounds from the gas phase to the water phase. It is also necessary
to be able to maintain as many active microorganisms as possible. It is known that
nearly only the outside of the biolayer is responsible for the biodegradation of
pollutants. This is owing to the restriction of oxygen and compounds diffusion
through the biolayer. The void volume is necessary in order to maintain as long as
possible the waste gas in contact with the medium. The removal of compounds with
high Henry's constants from an air stream is highly dependent on the mass transfer
and needs therefore a long retention time in a bioreactor.
Besides surface area and void volume the gas velocity can be of importance.
The gas velocity through the media affects the resistance of the layers of media. A
higher gas velocity leads to a higher resistance (i.e., pressure drop). Low resistance is
required because otherwise energy costs for the blower can reach up to 40% of the
total operational costs of a biological air treatment installation (Bioway, data not
shown). Often high gas velocities through a bioreactor are possible when air streams
contain low pollutant concentrations. When the overall removal of pollutants is not
being affected by creating a more or less open structure in the medium the
operational costs can be influenced significantly. So, media compositions can be
adjusted to the different types of air streams for different reasons. The most
important reason for changing medium composition is that it allows modifying the
surface area, the void volume and the resistance ofthe medium.
4.5 pH CONTROL
In bioreactors sodium hydroxide is not often used to control the pH. When
using caustic soda, recirculation of the process water in the biological air treatment
installation is preferable. However, as discussed earlier recirculation is not always of
interest to reach high purification efficiencies. Another disadvantage of using caustic
soda is that it may significantly affect total operational costs. Moreover, the use of
chemicals requires the application of specific safety rules.
Microorganisms active at a low pH may be used in bioreactors. Then, the
acids formed during the degradation process can be concentrated and removed with
water. Microorganisms active at a pH below 2 have been used in several bioreactor
applications. With such tolerant strains, relatively high concentrations of acids may
be produced, meaning that water consumption during bioreactor operation can be
reduced. In some industrial applications produced acids can be reused in the
production plant. If not, the running off water should be mixed with other water
streams. When other water streams are not available this running off water can be
neutralised with, for example, lime if necessary. So, using microorganisms adapted
to an extreme pH allows overcoming the disadvantages of using caustic soda for pH
regulation.
In some bioreactor applications the presence of ammonia in the air stream
alIows natural pH regulation. Ammonia dissolves in the water phase and forms NH4+
ions, capable of neutralising acid degradation products (sulphuric and nitric acids in
our applications).
When the process water is at a very low pH the measurements are often not
very ac curate as the pH scale is logarithmic. Therefore in some applications not only
the pH but also the salt content is measured. To determine the salt content water
conductivity is measured.
5.1 START-UP
For efficiently removing pollutants from a waste gas, the best available
microorganisms should be used. Because most of the waste gasses contain a mixture
of compounds a variety of microorganisms is mostly necessary to be able to degrade
aII the compounds. It is often thought that when the environmental conditions in a
biotreatment system are optimal microbial populations present in the waste gas or
Case study - New bioreactor 277
present on the (organic) medium wiII rapidly show up. Nevertheless, different
situations have shown that the growth of the optimal populations can take weeks or
even months (Chapters 3 and 4). It is important to ensure a good build up of the
biofilm on the media especially when the media are inorganic like in our bioreactors.
In our bioreactors inocula are always seeded on start-up. Biocultures capable
of efficiently degrading the compounds are used as inocula. Important parameters are
for example the ability to be active in a certain temperature range, at an extremely
low pH or, with a minimal use of nutrients. Start-up takes normally one to about four
weeks. During start-up, the process water is recirculated over the bioreactor.
Depending on the water source for the installation extra specific nutrients are used
during this growing phase of the microorganisms. Some factors like pH and
temperature can be of a large influence during the start-up. It has for example been
observed in one application that with only a few degrees (3 to 4 DC) temperature
increase the start-up period could be reduced from three weeks to one week.
6. Examples
Application
Settling tank of anaerobic water purification at a potato processing plant.
Airflow characteristics
• Flow: 250 m31h, temperature: 10-35 ec, humidity: 70-90%
• H2 S concentration raging from 400 up to 1000 ppmv
• CH4 concentration « 5% LEL)
• Odour compounds (fatty acids, organic sulphur compounds, ketones, aldehydes,
etc. )
278 N.JR. Kraakman
Type oJbioreactor
• PURSPRING system PS2150
• Footprint bioreactor: 2 m 2
• Built in 1997
Removal efficiencies
• H 2S removal > 98% (average over three years, measured daily first and measured
ones a week after the first three months)
• Odour removal > 97% (measured twice)
Application
Air from an anaerobic water purification plant at a brewery.
Airjlow characteristics
• Flow: 700 m 3/h, temperature: 15-25 DC, humidity: 60-80%
• H 2 S concentration ranging from 700 up to 1400 ppmv
• Odour compounds (organic sulphur compounds, fatty acids, mainly acetic acid,
ketones, aldehydes, aromatic compounds, terpenes, alkanes, mainly methane)
Type oJbioreactor
• PURSPRING system PS3250 (see Figure 12.2)
• Footprint bioreactor: 5 m 2
• Built in 1998
Removal efficiencies
H2 S removal > 97% (average over 1 year. measured daily).
Application
Sponge manufacturing process air.
Airjlow characteristics
• flow: 8500 m 3/h, temperatures 25-35 DC, humidity: 80-90%
• H 2S concentrations ranging from 200 up to 400 ppmv
• CS 2 concentrations ranging from 200 up to 400 ppmv
Type oJbioreactor
• V-SPRING system PS3400 (Figure 12.3)
• Footprint bioreactor: 15 m 2
• Built in 1999
Removal efficiencies
• H2S removal > 90% (average over 1 year, measured twice a day)
• CS2 removal > 75% (average over 1 year, measured twice a day)
Case sludy - New hioreaclor 279
Figure 12.3. V-SPRING bioreactor treating off-gases from a sponge mallufacturing plan!.
Application
Municipal waste water treatment plant.
Airflow Characteristics
• flow: 500 m 3/h, temperature: 5- 35 ec, humidity: 50- 90%
• H2S concentrations up to 300 ppmv
• Odour compounds
Type oJbioreactor
• ZEROCHEM-unit ZC1850 (Figure 12.4)
• Footprint bioreactor: 3 m 2
• Built in 1999
Removal ejjiciencies
H2S removal > 99% (average over three months during the summer period, on-line
measurement). See Figure 12.5 for H2S removal during day and night.
280 N.J R. Kraakman
A list of aII bioreactors that have been built and operated successfully is
presented in Table 12.1. It can be seen that some of the bioreactors have been
operating in the field for many years now. The number of applications is growing
and it is expected that many more bioreactors will be built in the near future.
Information on the investment and the operating costs of a bioreactor system
is presented Table 12.2. The costs are compared with other conventional techniques
like chemical scrubbing, incineration, adsorption and conventional biofilters.
7. Future developments
Each kind of industrial appIication needs a tailor made solution. As describe above
three types of bioreactors are standardised for specific applications. Future
developments will focus on many other applications. One of the developments is the
ability to increase removal efficiencies of very poor soluble compounds. Because of
the abiIity to operate the bioreactors in different ways to obtain optimal process
control this is one ofthe future development that is necessary.
Case study - New bioreactor 281
Table 12.1. List ofbioreactors that have been built and operated successfully
AIRFLOW
RAlE IMPORTANT YEAROF
PROJECTS (m 3fh ) COMPONENTS INSTALATION
Waste water treatment plant 500 H2S,odour in progress
Liftstation off-gas 500 H2S,odour in progress
Waste water treatment plant 250 H2S,odour in progress
POTW off-gas 2000 H2S,odour In progress
Waste water treatment plant 250 H2S,odour in progress
Sponge manufacturing process air 50000 H2S, CS 2 in progress
Waste water treatment plant 700 H2S,odour 2000
Rayan manufacturing process air 12500 H2S, CS 2 in progress
Waste water treatment plant 800 H2S,odour 2000
Brewery ground water processing off-gas 34000 H2 S 2000
POTW off-gas 1700 H2S,odour 2000
Oii production plant 2500 H2S (up to 1500 ppmv) 2000
Sewerage 500 H2S, adour 1999
Waste water treatment plant 500 H2S,odour 1999
POTW off-gas 4000 H2S,odour 1999
Table 12.2. The investments and the operating costs of a bioreactor system compared with other air purification techniques.
Based on an air stream of 8500 m 3/h with 50 ppmv H2S
H2S REMOVAL
ZEROCHEM-BIOREACTOR
300,---______________________________________,30
250~-----------------------------------------t25
UJ •••• • • (1)
~ 200fWl~._~------~~~~----_,~~~~~·~--~20 ~;
~~
~ ~
~
~ Q.
a
UI..... 150 15 B5"""::
~~ ~~
u~ 8~
UlM 100 10 o
(l)N
~ ~ ~
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....")~~~IO'?~o)'Y~--;~°!j'Y<;)rţ'?°?j'Yc'\.'?~c:5'Y~~~~'Y~.'?~<S'Y~rţ'?O...;~'!i'?(')l6ftO~~...;'Y~'?'?~(cj'Y~qj'?~...;'Y~'"'J'?0oţ'YCl~'?()'\.'Y<:;:).
T1ME
References
Alonso, C., Zhu, X., Suidan, M.I., Kim, B.R. and Kim, B.R. 1998. Modeling of the biodegradation
process in a gas phase bioreactor - estimation of intrinsic parameters. In: Proc. Conference on
Biofiltration. Reynolds F.E. (ed.), Tustin, California.
Cox, H.H.J. 1995. Ph.D. Dissertation, State University of Groningen, Groningen, The Netherlands.
Cox, H.H.J. and Deshusses, M.A.. 1999. Chemical removal of biomass !Tom waste air biotrickling
filters: screening ofchemicals of potential interes!. Water Res. 33: 2383-2391.
Cox, H.H.J., Nguyen, T.T. and Deshusses, MA 1998. Pollutant biodegradation in biotrickling filtes
revisited. In: Proc. Conference on BiofiItration. Reynolds F.E. (ed.), Tustin, California.
Cox, H.H.J., Nguyen, 1.1. and Deshusses, M.A. 1999. Predation of bacteria by the protozoa
Tetrahymena Pyriformis in toluene-degrading cultures. Biotechnol. Le!. 21: 235-239.
Groenestijn, J.W. van and Hesselink, P.G.M. 1993. Biotechniques tor air pollution control.
Biodegradation. 4: 283-301.
284 NJR. Kraakman
Heiningen, W.N.M. van, Kraakman, N.J.R., Gerbcns, S. and Groenestijn, lW. van. 2000. The
development of a biofilter system using fungi on inert carner material in combination with mites. In:
Proc. Conference on 13iofiltration Reynolds VE (ed ), Tustin, California
Heslinga, D.e. and Groenestijn, J.W van. 1997. "Jbennophilic biological wastc gas cleaning. In: Proc.
Intem. Symp. Biological Waste Gas Cleaning. Prins W.L and van Ham 1 (eds.). VDI Verlag GmbH,
DUsseldorf, Germany.
Kraakman, N.J.R., Groenenstijn, J. W. van, Koers, B. and Heslinga, D.C. 1997. Styrene removal using
a new type of bioreactor with fungi. In: Proc. Intem. Symp. Biological Waste Gas Cleaning. Prins
W.L and van Ham] (eds.). VOI Verlag GmbH, Diisseldorf, C;cnnany
Melse, R. W. and Kraakman, N.J.R.. 1998. Biological treatment of waste gases containing !I,S and CS 2
combined with the production of concentrated NaOH and H,S04' Meded. Fac. Landbouww. Gen!. 63:
1841-1847.
Picioreanu, C., Loosdrecht, M.e.M. van and Heijnen, 11 1999. Discretc-differential modelling of
biofilm slructure. Water Sci. Technol. 39: 115-122.
Seignez, e., 13odart, V., Lombardot, T., Stettler, M., Thoeni, C., Peringer, P and I1011iger, C 2000. A
biotrickling filter to treat chlorobcnzene-contaminated waste gas: Inoculum production, performance
and bacteria involved. In: Proc. 4lh International Symposium Environmental Biotechnology. IIartmans
S. and Lens P. (OOs.), Noordwijkerhout, The Netherlands, pp. 105-108.
Song, J. and Kinney, K.A. 2000. Effect of vapor-phase bioreactor operation on biomass accumulation,
distribution, and activity: linking biofilm properties to bioreactor perfonnance. Biotechnol. Bioeng. 68
50S-S I Ii.
Woertz, J.R., Kinney, K.A., Mclntosh, N.D.P. and Szaniszlo, P.J. 2001 1 Air Wastc Manage. Assoc.
(in press).
CHAPTER 13 BIOSCRUBBER FOR TREATING WASTE GASES
FROM WASTE WATER TREATMENT PLANTS
1. Introduction
The need to prevent public nuisance, particularly for installations near residential or
tourist areas, means that there is an increased need for the control of odour emissions
from waste water treatment plants (WWTP). Consequently odour emissions must be
reduced through the use of a better technology and cleaning of the resulting
emissions.
In waste water treatment, odour nuisances typically arise in the sewerage
system and at the waste water treatment plant, particularly at the inlet works and in
sludge treatment facilities. Problems are primarily caused by volatile sulphurous
compounds such as hydrogen sulphide and mercaptans. By covering and ventilating
the critical sections of the plant it is possible to create a satisfactory working
environment. However, it is often necessary to remove the odorous substances from
the ventilation air to avoid nuisances in the neighbourhood.
The waste water treatment plants Lynetten and Damhusaaen are owned and
operated by the partnership Lynettefaellesskabet IlS. The plants treat waste water
from eight owner municipalities. In total the plants treat approximately 275000 m3/d,
which is a population equivalent of 1.1 million. During the period 1991-97, both
treatment plants were extended to include nutrient removal. The costs of the
extension amount to f 160 millions.
The Damhusaaen WWTP treats sewage from a population of 226000 (350000 PE).
Primary treatment comprises 6 mechanical screens, 2 aerated grit and grease
chambers and 7 circular primary sedimentation tanks with a hydraulic capacity of
28000 m3/h. The screens and the grit and grease chambers are covered and
ventilated. The combined biological and chemi cal waste water treatment (Bio-
Denipho with simultaneous precipitation) takes place in four lines comprising
anaerobic tanks and aeration tanks having a total volume of 80000 m 3 . Final
sedimentation takes place in twenty-four circular tanks with a hydraulic capacity of
10000 m 3/h. The waste water is discharged into the Sound via a 1.5 km long pipe.
Primary sludge is digested in four digesters totalling 7600 m 3 and then dewatered
together with the secondary sludge in four lines comprising drum screens and
centrifuges. The produced gas is used to generate electricity and heat. The dewatered
sludge is transported by lorry to the Lynetten WWTP for drying and incineration
together with sludge from Lynetten. The ash is deposited in an environmentally
approved landfill at Lynetten.
The works dates back to 1930 and has later been extended by stages. As the
built up area becomes larger, the residential area has come c1oser, which means there
are residences very c10se to the plant.
As a result of the odour nuisances from the treatment plant, in 1992-93 a
survey was carried out to reveal the odour sources. The inlet structure, particularly
285
C. Kelllles alld M. C. Veiga (eds.), Bioreactorsfor Waste Gas Treatment, 285-298.
© 2001 Kluwer Academic Publishers.
286 N. G. Hansen and K. Rindel
the screen ing and the grit and grease chamber, tumed out to be the most important
odour sources at the treatment plant. It was therefore decided that measures should
be taken to reduce the odour emission from this area.
An aerial view of the Damhusaaen WWTP is shown in Figure 13.1. The inlet
works is seen in the middle, left hand section of the picture ne ar the circular primary
clarifiers.
The choice of the air cleaning method was based on considerations in relation to
operating costs, operational reliability, environmental friendliness, and space
requirement.
Case study - Bioscrubber 287
2. Plant description
passes. The amount of exhaust air is sufficient for produc ing a weak negative
pressure under the cover, thus taking care of both the process air used for aeration of
the chamber and atmospheric air taken in through openings in the cover.
2.1.2 Screens
The screens are covered with aluminium plates, allowance being made for access by
the staff in connection with service inspection and repair works (Figure 13 .2).
Ventilation is not taken directly from the screen building but from the inlet
chamber below the screen building, where a weak negative pressure is maintained.
By also establishing a weak positive pressure in the screen building, a reduction of
the exhaust air flow is obtained and with it a less expensive air c1eaning plant and a
better working environment for the staff.
The bioscrubber method combines two well-known processes: (i) an absorption unit
with inert media (a packed column) in which the pollutants are transferred to a liquid
phase; and (ii) a bioreactor based on the activated sludge principle in which the
pollutants are oxidised by means of microorganisms. A flow diagram of the
bioscrubber process is shown in Figure 13.3. The activated sludge from the
bioreactor is used as the absorption liquid in the column. Thus the two sub-processes,
mass transfer and biological oxidation, take place in separate but interconnected
units, simplifying the dimensioning and operat ion ofthe plant.
The absorption column contains an inert plastic or metal packing which
provides maximum contact between the air and the liquid phases and well defined
and predictable flow conditions. Before the c1ean air is released to the atmosphere. it
passes through a demister, in which liquid droplets are separated from the air.
filler
P1 NaOH
95
90
x
L= 32 m 3j(m2 .h)
85 +.--------.-------~--------~------~
0.50 0.75 1.00 1.25 1.50
Air velocity (m/s)
Figure 13.4. Influence of liquid load L on the cleaning efficiency for hydrogen sulphide.
Packed height = 6 m, pH = 8.5.
100
~
90
tf<
'--'
>-. 80
g 70
v
'u 60
}5
v
gp 50
'S
CIj
40
v
O 30 .
20 -
0.50 0.75 1.00 1.25 1.50
Air velocity (m/s)
The bioscrubber at Damhusaaen WWTP (Figure 13.6) was commissioned during the
latter part of 1996. The bioscrubber is made of stainless steel and operates
automatically as an integral part of the SCADA system (Supervisory Control And
Data Acquisition) ofthe waste water treatment plant.
It was required that the air leaving this particular plant should be as odourless
as possible. The air from the bioscrubber is therefore treated in a polishing filter to
remove any remaining odorous substances of low water solubility, which are not
Case study - Bioscrubber 291
absorbed in the scrubber section. The polishing filter conta ins an adsorbent. As most
of the polIutants are removed in the bioscrubber, the adsorbent has a long life
expectancy, thereby ensuring economical operation.
Figure 13.6. Bioscrubber at the Damhusaaen WWTP. In front the gri! chamber.
Variation
80 , - - - - - - - -
70
60
~ 50
~J
<;\; 40
Ei
~ 30
o
20
la
o~~~~~~~~~~
o 100 200 300 400
:-.Jumber Dt days 1'rom start
The Oxygen Uptake Rate (OUR), i.e., the oxygen consumption during the
biological oxidation (and endogenous rcspiration) in terms of the suspended solids
(SS) concentration was dctermined both with and without addition of a carbon source
(acetate) and with addition of sulphide. A fast adaptation of the sludge to the
sulphide was seen which, after a period of time, was oxidised 5-10 times the original
rate in unadapted activated sludge.
The tests with and without acetate showed that readily biodegradable organic
substances were not present in the samples and that the activated sludge only slowly
degraded acetate after a lag time. This indicated that the activated sludge contained
fewer heterotrophic microorganisms than normally, prcsumably owing to a low
content of organic matter in the air.
Case study - Bioscrubber 293
Therefore, it was not necessary to seed with speciali sed bacterial strains for
this application. This was also the case with regard to other applications of biological
air cleaning plants where native compounds were to be treated. In most cases, it will
be an advantage to start with a mixed culture as it is more robust than a specially
prepared culture. Furthermore, in many applications a specially prepared culture will
be difficult to maintain, as the introduced air is not sterile. Only in cases where non-
native compounds such as chlorinated solvents are treated, it seems an advantage to
use specially prepared microbial cultures.
3. Process experience
After more than four years' operation of the bioscrubber, the following important
experience has been gained.
3.1 START-UP
Start-up ofthe plant was rapid and straightforward because the activated sludge from
the aeration tanks was used as seeding material. This means that seeding with special
cultures was not necessary.
The cleaning efficiency is high, > 99 % for hydrogen sulphide in the scrubber section
alone with inlet concentrations of up to 75 mg H2S/m 3 . Outlet concentrations lower
than 0.1 mg/m 3 are easily obtained with the polishing filter in operation. Organic
294 N. G. Hansen and K Rindel
sulphur compounds only appear at low concentrations and are reduced to less than
0.1 mg/m 3 through the plant. The ave rage hydrogen sulphide load is about 10 mg/m 3
on an annual basis and approximately 25-35 mg/m 3 during the summer and autumn.
The pressure drop of air in the scrubber section is stable, which means that there is
no uncontroUed biomass growth on the plastic packing and therefore no risk of
clogging. This is a result of the low growth rate of the sulphide oxidising bacteria
combined with the continuous recirculation of scrubbing liquid.
3.4 pH MEASUREMENT
3.5 MAINTENANCE
The consumption of sodium hydroxide for neutralising the produced sulphuric acid is
stoichiometric (2.4 kg NaOH/kg H2 S) in relation to the amount ofhydrogen sulphide
absorbed at a pH level of 8.5-9.0 in the scrubber liquid. This means that no carbon
dioxide is absorbed from the air, which would have meant a higher consumption of
chemi caIs - as is the case in chemical scrubbers which are operated at a higher pH.
The consumption of adsorbing agent in the polishing filters depends upon the
content of substances with low solubility in the ventilation air, because, in practice,
aU the hydrogen sulphide is removed in the scrubber section. Fresh adsorbing agent
added in March 1998 was not exhausted until October 1999. Therefore, the
consumption can be expected to be approximately 400-500 kg/year. As the pollutant
load during winter is rather low, fresh adsorbing agent was not added until April
2000 and it stiU did not show any sign of exhaustion in November 2000.
It is to be expected that foaming might occasionaUy occur in the sludge
suspension. To prevent foaming, an antifoam agent is dosed into the bioreactor.
Dosing takes place discontinuously in predetermined amounts controlled by a timer
function. The average consumption is about 1 l/d. Furthermore, a foam sensor placed
above the liquid surface in the scrubber section activates the dosing pump in order to
suppress any uncontrolled foaming.
Case study - Bioscrubber 295
The operating costs for the bioscrubber are only about half those for a chemical
scrubber at inlet concentrations of about 10 mg H2S/m3• This is mainly owed to the
lower consumption of chemicals, because the oxidising agent of a chemical scrubber
is replaced by microorganisms in the biological process, and the near-stoichiometric
consumption of sodium hydroxide in the bioscrubber. The higher the inlet
concentration, the more advantageous the biological process. Therefore, at an inlet
concentration of 50 mg H2S/m3, the operating costs for the bioscrubber are as low as
one fourth of the operating costs of a chemical scrubber. Figure 13.8 illustrates this
for two different inlet concentrations.
The comparison is based on a one-stage bioscrubber with a polishing filter
placed downstream and a traditional two-stage chemical scrubber with an acid first
stage used for removal of nitrogen compounds (which may otherwise cause
undesirable side reactions in the next stage), and a basic and oxidising scrubber
section utilising sodium hypochlorite.
1.4
scrubber
1.2
.~
ao 0.8
o
8
4l 0.6 Chemical
.... scrubber
'"
o 0.4
U
0.2
o
Low inlet concentration High inlet concentration
~ Power ~ Chemicals o Water lllllI Maintenance
Figure 13.8. Operating costs of a bioscrubber and a chemical scrubber. Low inlet
concentrations correspond to 10 mg H2S/m1 and 3 mg org.S/m1, high inlet concentrations
correspond to 50 mg H2S/m1 and 3 mg org.S/m1 •
In the summer period of 1997, complaints were received of odour being a nuisance to
the neighbourhood of the waste water treatment plant. The Lynettefaellesskabet
contacted the Environmental Control Body (Miljokontrollen) in Copenhagen, which
is the supervising authority for the plant. It was agreed that the Body should make a
number of odour observations in the are a in the periods October 1997 to February
1998 and May 1998 to September 1998. The observations, which were made in the
plant lee side in radii of 200 m and 400 m respectively from the primary treatment
(potentially the largest odour source), where also the bioscrubber is located, were
characterised as eno odour', 'noticeable odour which, however, does not justify
complaints' and 'excessive odour'. The total number of observations amounted to
138 in the first and 149 in the second period, each period reaching a twenty days
duration.
A survey of the vicinity of the plant revealed a number of potential odour
sources, which were not generated by the Lynettefaellesskabet. The sources in
question were three pumping stations, a sludge receiving plant and a combined sewer
overflow. There are other potential odour sources in the area, for example, a
composting plant is located nearby. The results of the odour observations are given
in Table 13.1 (Miljokontrollen, Copenhagen, 1998).
Table 13.1. ResuJts of odour observations in the neighbourhood of the Damhusaaen WWTP
May 1998-
Sept. 1998 136 13 O 91 9 O
Based on the survey, it was concluded that Damhusaaen WWTP did not emit
any noticeable odour during the test periods.
4. Future measures
Similar covering of the grit and grease chamber at Lynetten WWTP (750000 PE) is
intended. In addition, the overflow channels in the primary sedimentation tanks will
be covered. The covering is made partly for the sake ofthe working environment and
partly to avoid odour being a nuisance to the adjoining site, which no longer houses a
ship building industry but other activities such as a drive in cinema. To begin with,
the discharges from the screens and the grit and grease chamber are collected, and
Case study - Bioscrubber 297
5. Conclusions
1. Covering and enclosing the critical sections such as grit and grease chamber and
screens at the inlet to the Damhusaaen WWTP, together with cleaning of the
ventilation air, have reduced the odour emissions to a level of practically no
noticeable odour nuisance to the treatment plant neighbourhood.
3. Experience from more than two years of operation has shown that the
bioscrubber can be characterised as follows:
(a) Environmentally friendly process without the use of oxidising chemicals;
298 N. G. Hansen and K. Rindel
(b) High cleaning efficiency with respect to hydrogen sulphide and organic
sulphur compounds;
(c) Low operating costs owed to low consumption of chemicals. Operating costs
are halfto one quarter ofthose of a chemical scrubber at inlet concentrations
in the range of 10-50 mg H2S/m3;
(d) Small space requirement at larger air flows owed to the relatively high
velocity ofthe air through the scrubber;
(e) High reliability as drying out, acidification, clogging and accumulation of
reaction products do not occur;
(i) Maintenance requirements are relatively low, because the process can be
widely automated;
(g) Quick start-up with ordinary activated sludge from a waste water treatment
plant;
(h) On the basis of simple design rules, the process can be designed in an
optimum way for the given amount of air and concentration of pollutants; and
(i) Suited to removal of acidifying substances without any negative effect on the
life of the plant.
Acknowledgement
References
Hansen, N.G. and Rindel, K. Recent experience with biological scrubbers for air pollution control in
Denmark. In: Biotechniques for Air Pollution Abatement and Odour Control Policies. Dragt AJ. and
van Ham J. (eds.). Eisevier, Amsterdam, The Netherlands, 1992, pp. 143-154.
Heist, J.H., Hansen, N.G. and Rasmussen, H.H. Control of odor emissions from wastewater treatment
plants in a bioscrubber. In: Proc. Water Environment Federation 68 1h Annual Conf. & Exposition,
Water Environment Federation, 1995, Alexandria, VA.
Milj0kontrollen. 1998. Odour survey in the surroundings of the Damhusaaen wastewater treatment
plan!. The Environmental Control Body in Copenhagen, (in Danish).
Rasmussen, H.H., Hansen, N.G. and Rindel, K. 1994. Treatment of odorous nitrogen compounds in a
bioscrubber comprising simultaneous nitrification and denitrification. VDI Berichte. 1104: 491-497.
Van Lith, c., Leson, G. and Michelsen, R. 1997. Evaluating design options for biofilters. J. Air Waste
Manage. Assoc. 47: 37-48.
Williams, T.O. Biofiltration for control of odorous emissions and volatile organic compounds from
wastewater and sludge processing facilities. In: Proc. WEF Specialty Conf. on Odor and Volatile
Organic Compound Emission Control for Municipal and Industrial Wastewater Treatment Facilities,
Water Environment Federation, 1994, Alexandria, V A, pp 4.1-4.13.
CHAPTER 14 ODOUR CONTROL AT WASTE WATER
TREATMENT PLANTS BY DIFFUSION
INTO ACTIVATED SLUDGE BASINS
1. Introduction
Diffusion of odorous air into activated sludge bas ins has been practised for over 30
years as a technique for controlling odours at waste water treatment plants. At least
25 facilities in North America currently use or have used this approach. Table 14.1 is
a list of these plants with information on sources of odorous air, year of installation,
foul air flowrate, and problems experienced.
2.1 CORROSION
Concern for cOITosion of activated sludge blowers has generally impeded more
widespread use of the odour diffusion technique. While some plants have reported
cOITosion of blower inlet components such as filters or silencers, documentation of
cOITosion of the internal workings of the blower is very limited. Two plants reported
cOITosion of stee1 inlet guide vanes. In one of those cases, the carbon steel vanes
were replaced with nickel plated vanes with no further problems. At the other
facility, introduction of acidic condensate was suspected as the cause of corrosion as
there was no moisture trap upstream ofthe blower. At a minimum, a demister should
be inc1uded before the blower to remove acidic droplets or condensate formed
upstream in the ductwork. All inlet components should be of corrosion-resistant
material such as 316 SS. Some new facilities have specified nicke1 plated internal
blower components or a corrosion-resistant synthetic resin coating.
Many facilities practising odorous air diffusion have reported the accumulation of a
'tar-like substance' or 'greasy film' on the internal components of the blowers. No
information is available on the chemical make up of this substance. It is likely from
grease aerosols that become 'baked' onto the blower components at the e1evated
internal temperatures. Most plants remove this material by steam c1eaning, and one
facility installed steam injection ports on the blower housing. An industrial waste
water treatment plant uses household over c1eaner to remove the film. One plant in
Los Angeles County, California reportedly solved the problem with installation of a
two stage air filtration system.
299
C. Kelliles alld M. C. Veiga (eds.), Bioreactors for Waste Gas Treatment, 299-305.
© 2001 Kluwer Academic Publislzers.
Table 14.1. Summary ofselected facilities in North America using activated sludge diffusion for odour control
"'2"
Treatment plant Plant Source of Yeac Odorous
and location capacity adour controlled installed airflow Comments
ml/d m'jmin
(mgd) (cfm)
Banny Brook WWTP 500 Fennenters for BNR 1994 40 Corrosion cfinlet filters occurred, caus ing damage to blower. New guide vanes are nickel-plated.
CaIgary, AB (130) process (1400)
Kyrene Water Reclamation Aerated equalisation tank 1993 150 FRP fan transfers foul air ta centrifugal blowers for diffusion via jet aerators High H1S ( > 50
Facility (3)
" (5400) ppmv). No corrosion problems reported
Tempe, AZ
Las Coyote WWTP 140 Primary clarifiers 1970 280+ Filters cleaned every 6 months. Blo\\'ers rebalanced and c1eaned every year. No corrosion reported.
Cerritos, CA (37) Influent wet \vell (10000+) Coarse bubble ditTusers. Steel blowers w/coal tar epoxy. SS ducting
~
Long Beach WWTP 95 Primary c1anticr 1973 170+ No filters 011 compressor suction. Have to steam clerul suction and compressor once a ycar Coarse
~
Long Beach. CA (25) (6000+) bubble diffusers: no c1oggmg. Concrete corrosion. 100% removal ofH 2S
0
Hyperion WWTP 1140 Headworks 1959 5100 Have had to c1ean blowers twice since start-up. Fine bubble ditfuscrs. No corroslon rcported. lJ:j
a
Las Angeles, CA (300) Primary c1arificrs ( 180000) Clean plus raul air pass through ane systcm Estimate adaur removal efficiencies 96-99%, VO(· ~
;.;-
DAF thickencrs removal 80%. No Ion ger practlsed after con vers ion ta pure oxygen activated sludge ...,
'"
Emuent pumr statian
LA Glendale WWTP 76 Bar screens 1976 570 Originally coarse bubble dltfusers. From 1979-1991 transitioned to fine bubblc No corrosion or
Las Angeles, CA (20) Influent pumr station (20000) clogging reported. Foul air IS only souree of air ta aeration tanks.
Primaries
Tennmal Island WWTP 80 Headworks 1977 850 Fine bubble difrusers; steel blo\l,'er; PVC piping. No plugging. COlTosion only of concrete in
Las Angeles, CA (21) Primary dariliers (30000) covered tanks.
Centrifuge bldg
Sludge blendl!lg tank
TillmanWWTP 150 Primary c1arilicrs 1984 Fine bubb1c ditfusers. no clogging. No cOlTosion reported
Las Angeles. CA (40) Sase of scrc\\ pumps
Bar screens
PO!TIonaWWTP 49 Primary c1arifiers 1965 170+ Fine bubble diffusers. Chatlge filters quanerly.
Pomona CA (13) (6000+)
Table 14.1. (Continued)
Lawell WWTP 120 Gravity thlckeners 1984 260 Switched from caarsc 10 tine bubble diffusers In 1991. AII SS piping. ~o fillcrs. Same parllculate
Lowell,MA (32) Siudge dc\\atering (9000) build-up al dlffuser hrads
Springfield Regional WWTP 250 In-vesselwmpostlllg NA 130 Interim measure beforc construction ofthennal oxidiser SS coarse bubble diffusers, Impellcrs
Springfield, MA (67) (4500) coated w/s)'nthetic re"ln SS and HDP piping: ilO corrosion or plugging
Scarborough WWTP 6.8 Aerated sludge holdmg 1983 2.8 Foul air is separate s~ . . tem from clean air supply; coarse bubblc diffusers, steci blower Conosion
Scarborough, ME (1.8) tank (100) only an DI intake plpC) and steel inlet silencer v..,
<::>
......
Table 14.1. (Continued)
""~
Treatment plant Plant Souree of Year Odorous
and locatien capacity odour control led Înstalled airtlow Comments
ml/d m3/min
(mgd) (cfrn)
Concord WWTP 39 Siudge holding tanks 1994 20 Interim solutian until scrubbers built in 1996. High adour and H2S levels to aeration. Fine bubblc
Concord, NH (102) (700) diffusers performed better than coarse. No corrosion after 2 yr.
Concord WWTP 39 Intluent channels, grit 2000 71 Perfonnance data to be collected in 2001
Concord, NH (102) chamber, primary clarlfier (2500)
launder
Durham WWTP 9.S Siudge holding tanks 1993 37 COITosion of steel înlet filter; replaced with SS. Fine bubble diffusers; no plugging. Foul air is 100%
Durham, NH (2.S) (1300) of aeration air
Roche Chemi cais II Primary clarifier 4S0 Industrial WWTP, Coarse and fine bubbIc diffusers; condensate traps; tar-Iike substance 011 blowcr
Belvedere, NJ (3) (16000)
~
impellers "'"
o
Musonetcong WWTP 9.5 In-vesse! composting 1992 140 Coarse bubble diffusers. 2 m (6 ft) deep strictly for odour control (basins are mechanically aerated)
Stanhope, NJ (2.5) (SOOO) B10wers have syllthetic resin coatmg on impeJlers. heads, and sections
~
~
Newberg,OR 15 In-vesscl composting 1988 68 Oedicated system for diffusion of odours into oxidation ditch; coarse bubbIc ditfusers; 110 corraSlon ~
....
(4) (2400)
Valley Forge WWTP 30 Influent structure 1996 62 Dcdicated fine bubble diffuser system for adour control, Aeration tanks mechanically aerated High
Phoenixville, PA (8) Primary clarifiers (2200) inlet I-{zS. 'Tar' build up caused conventional PO blowers to shut down Intake duct and tilter
modifications soIved problems.
Walnut Creek WWTP 230 Headworks 1977 1060 Fine bubble diffusers Filters on blower intake. No corrosion reported. Fibreglass fans transICr air ta
Austin, TX (60) Primary clarifiers (37500) blower plenum. 'Greasy' film on bIower Iabes removed with steam
Flow equallsation
Sewer tUHnei
Trinity River Central WWTP 615 Raw sewage PS 1997 510 Fine bubble dîffusers Filters on intakes of centnfugal blowers. Now used as back up to biofilter
Headworb. Pri, clar systern
Dallas, TX (162) (18100)
efflllent channel
Gravity th ickeners
Sludge holding tanks
Arlington Ca. WPCP 110 Headworks 1995 570 SteeI blowers, coarse bubble diffllsers, No corrosion problems. Regular inspection program jor
Alexandria, VA (30) (20000) blower alignment, oii change.
Case Study ~ Activated sludKe diffusion 303
The waste water treatment plant in Concord, New Hampshire used activated sludge
diffusion as an interim measure to control odours from a sludge holding tank. The air
from the headspaee of the holding tank was pulled through an existing positive
displacement blower and diffused into a meehanieally aerated activated sludge tank
at approximately 37 m 3/min. Coarse bubble diffusers were first tested. As shown in
Table 14.2, removal of odour (as measured in dilutions to threshold or odour units)
was over 96 pereent, but odour conccntrations at the surface of the aeration tank were
almost 50 times background levels. Hydrogen sulphide concentrations were also
elevated well above background concentrations. The same test was conducted using
tubular, flexible membrane, fine bubble diffusers. Odour and H2 S removals improved
dramatically sueh odour and H2 S concentrations at the surface were reduced to the
background leve1s measured when no foul air was introduced.
Table 14.2. Performance of activated sludge diffusion for odour control at Concord, New
Hampshire, USA
Odour coneentration
HzS, llllmv
O/T,O.U.
Odour Souree
Back- Back-
In Out In Out
Ground Ground
Sludge holding tank
Coarse bubble 24150 850 10 ~100 7.8 0.2
Fine bubble 39000 18 14 ~100 0.3 0.2
In the year 2000 the Concord waste water treatment plant replaeed the
existing mechanieal aerators with fine bubble diffusers and used the new blower to
diffuse foul air. The blower receives 100 pereent foul air from the influent channels.
aerated grit chamber, and primary clari fier effluent launders. The system is etIective
and no problems have been reported. Since the plant uses biotowers upstream of the
aeration tanks for BOD reduction, the demand for oxygen in the aeration tanks is
relatively low. As a result blower air flow rates have only been 260 to 530 m 3/min,
less than the design foul air flow of 660 m 3/min based on a ventilation rate of 6 air
changes per hour from the covered odour sourees. Performanee testing of the odour
diffusion system is scheduled for the summer of 200 1.
The 30 MLld Valley Forge plant had experienced high odour emissions from the
turbulent influent chamber, primary clarifier feed wells and effluent launders, and
primary effluent distribution ehamber. Hydrogen sulphide concentrations at turbulent
surfaees were 50 to 500 ppmv in the air. The sewer authority chose activated sludge
diffusion over chemi cal scrubbers or other odour treatment alternatives. even though
the activated sludge tanks were meehanically aerated. A dedicated system of blowers
and diffusers was installed in 1996 to treat 62 m 3/min of odoraus air. Design criteria
are summarised in Table 14.3.
304 R.P.G. Bowker
Table 14.3. Key design criteria for odour control system at Valley Forge WWTP
Parameter Value
Odour sources Influent chamber
Primary claritier feed wells
Primary claritier effluent launders
Primary effluent splitter box
Air flow 62 m3/min (2200 cfm)
Air exchange rate below covers 12AC/hr
Inlet H2S (estimated) 120 ppmv (summer)
Blowers 2--45 kW (60 hp) positive displacement
Diffusers 394 tubular, flexible membrane type at
4.3 m (14 fi) depth
Materials of construction Covers FRP
Ductwork PVC, 316 SS
Blower tilters, silencers 316 SS
Blowers steel
Discharge piping 316 SS
Concrete protection Epoxy coating above water line
Performance data are shown in Table 14.4. The system was effective in
reducing odours and H2S levels at the surface of the aeration tanks to background
levels. During the tirst year, problems were experienced with accumulation of
organic matter in the positive displacement blowers that caused the blowers to shut
down. This was attributed to suction piping being too close to the surface of the
covered primary claritier feed well, causing grease to be pulled into the blower, and
to an inefticient tilter system. Afier these problems were corrected, the system has
provided reliable service. However, the epoxy coating used to protect the concrete in
the covered tanks failed in the presence of sulphuric acid.
Table 14.4. Performance of activated sludge diffusion for odour control at Valley Forge
WWTP, Pennsylvania, USA
Odour concentration
HzS, ppmv
D/T.O.U.
Odour Sources
Back- Back-
In Out In Out
Ground Ground
Influent chamber, primary 19000 5 5 77 0.1 0.05
claritier feed wells and 7 30 0.1 0.1
effluent launders,
distribution box
Case study - Activated sludge difJusion 305
Power costs for a dedicated odour diffusion system are high, and may make
use of a dedicated blower and diffuser system uneconomical compared to other
alternatives. According to Valley Forge staff, however, mechanical aerators that are
elosest to the foul air diffusers are now operated at low speed, and no net increase in
power consumption has been experienced.
Table 14.5. Removal of reduced sulphur compoullds alld odour by activated sludge diffusion,
Ailnapolis WRF pilot study
A c1osed, 49,261-267
Absorption, 17,24-27,86, 134, 152 rotating, 202
Acetobacter sp., 246 Biomass retention time, see Siudge
Actinomycetes, 66 retention time
Activated carbon, 32-35, 62,67,88- Bioreactor,4, 17, 140-144, 152
90,248 Bioscrubber,5-7, 133-162,215,236
Activated sludge, 9, 115, 140,215-254 Biotrickling filter, 5-7, 99-131, 206-
Adsorption, 17,32-37,51,86,100, 207,246
115,218,233,261-263,282 Board industry, 7
Column,25 BoIton criteria, 184
Isotherm,34-37 Breakthrough curve, 36
Aeration, 140, 143, 153 Breweries, 278
Aerosol, 7,9, 133 BTEX, 4,88,186,219-220,228-229,
Air 233,240-241
Composition, 3 Bubble column, 219-221, 223-224,
Velocity, 50-51,136, see a/sa gas 242,245-246
velocity Burkholderia sp., see Pseudomonas
Airlift, 154,222-224,233,243-249 sp.
Alcaligenes sp., 70, 89 Butanol, Il, 88
A1gae, 73, 116 Butene, 185
A1kylbenzenes: 55,69-71, 78, 81-82
A1pha(a),218-219 C
A1pha-pinene, see Pinene Carrier
Ammonia, 3, 7-8, 73,75,82,88, 107, organic, 63
144-148,155,168,170,181,233, inorganic, 67, 73, 77-79
257-258,271,276,282 synthetic, 114
Anaerobic, 6, 79, 114, 147, 150-154, Catalyst, 39, 180
179,237-238,273,277-278 Celite, 61, Il O, 245
Andrews equation, 55, 60, 228 Cell
Animal rendering, 7, 148 composition, 74-75,142
Arrhenius equation, 112 counts, 66, 73-74
Arthrabacter sp., 90 Cellulose, 166
Centrifugal force, 19-20
B Ceramic, 26, 66, 78-79,89,224
Bacillus sp., 70,90 Channelling, 66, 68, 81, 83, 260
Backwashing, 124-125 Chemical industry, 7
Baghouse, 20 Chemical Oxygen Demand, 142, 143,
Bark, 64, 75, 83, 85, 88 146,191,239
Basidyomycetes, 69 Chlorinated compounds, 44, 186, 190,
BET equation, 36 194
Biofilm Chlarobium sp., 237
model, 57, 172-173 Clogging, 41, 82-84,100, 124-126,
thickness, 76, 121, 172,201 142, 145,202,217,235,283
Biofilter, 2, 5-7, 47-98,100,223,236 Coconut fibre, 258
open,49, 77,104,257-260 COD, see Chemical Oxygen Demand
308 Index
G Liquid,
Gas hold-up, 223 hold-up, 103
Gravity settling chamber, 18 velocity, 119-120, 137
Groundwater poliution, 6 Lithographic operations, 8
Growthrate(~),55-56, 120, 141, 173 Livestock, 156
Load celi, 79,263
H Loading rate, 51-53, 136,224
Haldane equation, 60
Hardboard manufacturer, 7 M
Heather,85 Maintenance, 120, 124, 141
Henry's law coefficient, 51,57-58, Mass transfer, 28-32, 122, 137-138,
107,109, 112, 133, 137-139, 170, 173-175,205-206,225-227
219-220,226,230 zone(~Z),36-37
H2S, 63, 80-81, 89, 99-100, III, 115, Membranes, 44, 166-168
134,147,151-154,157-158,232- Membrane reactor, 163-177
234,237-239,247,257,271,274, Mercury lamp, 180
271-279,281 Methanol, 51, 70, 75, 89,109, 112,
HTU, 31, 138-139 154,171,190,219,233,242,261
Humic acid, 65 Methyl-ethyl-ketone (MEK), 89, 148,
Humidification, 48, 77-78, 80 187
Hydrogen sulfide, see H2S Methyl-iso-butyl-ketone (MIBK): 89,
Hyphomicrobium sp., 88,242,246 144
Methyl-tert-butyl-ether (MTBE), 5,
1 107, 1I5-116, 163, 170
Incineration, 17,37-41,86-87,100, Methylosinus sp., 245
157, 188,261-262 Michaelis-Menten,
Inhibition constant, see K1 constant (K.o), 142
Inoculation, 68-71, 115, 142,259 equation, see Monod equation
Mist eliminator, see Demister
K Mobile sources, 2-3
K1, 55, 60, 120,228 Modeliing, 49, 54-62, 172-174,225-
Kinetics, 55-60, 120, 137, 183,227- 232
229 Moisture, see Water content
Kt, see kL Monod equation, 55-57, 60,120,141,
Kt,29-30, 138, 173,225 173,227-230
KL~ 122, 130,210-211,218-221, Mould,81
224-227 Mycohacterium sp., 88
Ks, 55-56,141,173,228,231
N
L Naphthalene, 230-231
Lacquering industry, 7, 9 Nitric oxides (NOx), 2, 8, 39, 65, 15 L
Lactic acid, 257 155, 157-158, 182,238
Langmuir isotherm, 36 Nitrogen compounds, 269
Lava rock, 99, 103, 111, 114 Non-steady state, 61, 123
Leather industry, 7 NTU, 31,138-139
Lift stations, 271 Nutrients, 63-68, 74-76,117-119,
Lignoceliulosic material, 69,72 142-144, 146,260
310 Index
o 203, 234
Odour,7-9,232-236,257,282 Polypropylene (PP), 104-105, 137,
definition, 10 166--170
Olfactometer, 12 Polystyrene, 64-66, 74, 83,90
Operating line, 28 Polysulfone, 167-168
Overall heat transfer coefficient (U), Polytetrafluoroethylene (PTFE), 166
43 Polyurethane foam, 64, 66, 115
Oxidation, see Incineration Polyvinyl chloride (PVC), 104-105,
Oxygen limitation, 76, 113, 128 136,202,234
Oyster shells, 82, 245 Porosity, 27, 32-33, 49-50, 65, 114-
115,169-170
p Power, 154, 187, 189-190, 22()""'221,
Packed tower, 26-28, 135 232,247,282
Packing, see Carrier plant, 154
Paint booth, 144 Predation, 102, 1l8, 121, 124
PalI rings, 26, 64, 72, 110, 114, 135 Pressure drop, 18-20, 26-27, 82-84,
Paracoccus sp., 239 100, 136, 163
Parts per million Pre-treatment, 10, 17,48,80,146,
definition, Il 179,258
ParticIes, 2-3, 7-8, 17-25,48,99, Process control, 105-106,276--277
133,189,217,247,258,262 Propene, 168, 170, 174
P articulates, see P articI es Protozoa, 65, 73,101,116--117,124
Peat; 64--68, 78-79, 88-90, 258 Pseudomonas sp., 55, 70, 89-90, 110,
Perchloroethylene (PCE), 69, 151, 1l7, 123, 151,240,244-245
182-185,187 Pu1p and paper industry, 8
Perlite, 53, 61, 64, 67, 72, 78-79, 83, Pulse Jet collector, 22
88-90 PVC, see Polyvinyl chloride
Permeabi\ity constant (K), 21
Phanerochaete sp., 69, 72 R
pH, 81-82, 105, III, 119, 133,258, Raschig rings, 26, 135
275-276 Rate equation, 54, 60
Phosgene, 38, 182 Rayon manufactures, 9, 281
Phospholipid Fatty Acid Analysis RBC, see Rotating Biological
(PLFA),73 Contactor
Photocatalytic oxidation, 181-184 Reaction
Photochemical, 10, 44 \imitation, 59-60
Photolysis, 10, 185-186 rate, 57-60
Pinene, 51,69-70, 72, 79, 89, 112 Recirculation, see Recycling
Plasma, 179, 186, 188 Recycling, 119-120, 146, 169,263
Plate column, 31 Refinery, 151
Plate counts, see Cell counts Refuse dump, 282
Plug flow, 57, 62 Removal efficiency, 53, 102, 204
Pollutants Rendering industry, 8
anthropogenic, 4 Resin production, 8
natural,4 Retardation factor, 50..... 51
Pollution Reverse f10w cIeanmg, 21 ..... 22
sources, 4-6 Reynolds number (Re), 18,208,211
Polyethylene (PE), 104-105, 137, 168. Rhodococcus sp., 70. 90, 242
Index 311
RNA, T
16S-rRNA, 73,117 Tabaco industry, 8
Rotating Biological Contactor, 5-7, Teflon, 166
201-214 Temperature, 32-33, 38-45, 80- 81,
Rotarional speed, 205-207, 210-211 112
Terminal settling velocity, 18
S Tetrachloroethylene, see
Sand, 64, 66 Perchloroethylene
Scanning confocallaser microscopy Thermophilic, 80-81, 112, 148, 154
(SCLM),122 Thiele modulus, 59-60
Scrubber, 23-25,111,133,135-136, Thiobacillus sp., 70,81,89, 106, III,
258,282,291 151,153,238-239,274,292
SEC, see Surface-specific elimination Ti0 2, 180-182, 184, 186, 191
capacity Toluene, 30-40, 51, 55, 63, 67, 72,
Shaker,21 75-76,81,88,90,107-110,121-124,
Silica gel, 33 144,148-149,151,167-169,190,
Site remediation, 4 212,220,226,231,233,241,243
SLO, see Surface-specific substrate Toxic, 5, 62,124, 141-142
load Trametes versicolor, 69
Sludge retention rime (SRT), 218, 221, Trich1oroethylene (TCE), 38, 107,
230,235,241 151,167,182,187,190,229,233,
Soil, 66, 79, 87-88 243-246,261
Soil Vapor Extracrion (SVE), 6 Trickling
Sonolysis, 191-192 density, see rate
Sparged suspended growth bioreactor, filter,47
219-222,224 rate, 102, 120, 136
Specific oxygen transfer efficiency Triethylamine, 90
(SOTE),217
Specific surface area, 68,135-136, U
163 UltraViolet (UV), 44, 136, 180, 185-
Sponge manufactures, 6, 278 186,190
Spray tower, 24, 135 Uplow Anaerobic Sludge Bed reactor
Start-up, 68-69,115-116,259,292- (UASB),151
293
Stationnary sources, 3 v
Storage tanks, 8 Vapour
Stripping factor, 139 concentration, II
Styrene, 69, 71-72, 77,89,109, 147, definition, 10
149,192-193 Vegetable oii production, 8
Sulphur compounds, 38, 69, 109, 147- Vehicles,4-5
148,257-258,269 Venturi scrubber, 24, 135
Superficial Vermiculite, 64, 66, 72
gas velocity, 51, 58, 83, 223 Virus, 65
liquid velocity, 119-120 Viscose industry, 271
Supply rate, 118 Void fraction, 26, 65
S urface loading rate, 51
Surface-specific elimination capacitv, W
204,207 Waste water, 26, 42, 68, 100, 165,281
312 Index