Renewable and Sustainable Energy Reviews 73 (2017) 892–903

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Renewable and Sustainable Energy Reviews

journal homepage: www.elsevier.com/locate/rser

Recent advancement in biogas enrichment and its applications MARK

⁎
Rahul Kadam, N.L. Panwar
Department of Renewable Energy Engineering College of Technology and Engineering, Maharana Pratap University of Agriculture and Technology,
Udaipur 313001, Rajasthan, India

A R T I C L E I N F O A BS T RAC T

Keywords: Production of biogas and its utilization has several environmental benefits. It is a source of renewable energy,
Biogas and its production is considered and manure producing factory. Biogas has wider industrial applications for this
Bio-CNG up-gradation is desirable. Up-gradation of biogas has drawn attention due to rapid increment in the price of
Enrichment fossil fuels. It has an open new window to replace natural gas. There are several up-gradation technologies are
Clean fuel
available and developed by many scientists. In this paper, attempts have been made to discuss various biogas
Anaerobic digestion
purification technologies, which are widely used all over the world and major technologies, which are under
development or research. The widely accepted technologies have been with more prominence on their
operation, merits and demerits and their future scope are also discussed.

1. Introduction g VS respectively after 10 and 28 days of digestion [6]. Municipal solid

Energy is the backbone of developing countries like India.
Conventional energy sources such as crude oil, coal and natural gas
are used to fulfill increasing demands, but these resources are
exhausting rapidly with pace of the time; worldwide primary energy
consumption has grown by 0.9% in 2014 [1]. It is clear that renewable
energy sources like biogas, biomass, wind and solar supply 14% of total
world energy demand [2]. Biogas is generated from anaerobic digestion
of organic compounds such as food wastes, cellulosic biomass, and
animal waste. Nowadays, it is not only used for cooking but also used
for vehicular operations and electricity generation. According to Agstar
report, anaerobic digestion plants have a capability to generate 13
million megawatt hour per annum in USA [3]. In India, Ministry of
New and Renewable Energy had set a target to achieve 48.55 MW
energy from biogas plants till 2022 [4]. There is the tremendous
potential in India as well as rest of the world in employing anaerobic
digestion as waste treatment method as well as an energy production
technology.
Anaerobic digestion is a series of biological processes, in which
micro-organisms breakdown of bio-degradable material in the absence
of oxygen. It involves a series of bio-chemical processes such as
hydrolysis, acidogenesis, acetogenesis and methanogenesis. There is a
lot of research done on variety feedstock for anaerobic digestion.
Methane yields from corn Stover, wheat straw and switch grass were
2–5 times higher than those farm yard wastes, waste paper had
methane yield of only 15 L/kg VS and pine had only 17 L/kg VS [5].
Food is also good source methane, which yields about 348 and 435 mL/
wastes also utilized for methane production, and it were found that
inoculums influence the performance of anaerobic digesters for treat-
ing municipal solid waste. The methane concentration increases with
inoculums which was 42.6% for 15% of inoculums [7]. Extensive
research is going on, in order to increase CH4 yield during anaerobic
digestion.
Biogas can be used for electricity production in co-generation or
combined heat and power (CHP). In biogas upgrading, methane in
biogas can be concentrated to the same standards as natural gas. It cab
ne injected into the household pipeline system for distribution. Under
cryogenic conditions, biogas is converted into compressed biogas or
liquid biogas. The technology can be used to upgrade biogas by chilling
the gas around −80 °c but usually cryogenic technology is associated
with the production of liquid biogas. Then the gas is further chilled to
−162 °c. Another product that often mentioned is liquid CO2 or LCO2
[8]. Besides that, biogas can be used as transportation fuel and, in
many countries filling stations are available with 100% methane or
blended with natural gas. An automated scrubbing based biogas
purification plant has been developed at IIT Delhi, India and the
enriched and bottled biogas have been regularly fuelled to a car [9].
Biogas can be reformed into cleaner fuels like syngas and hydrogen.
Nickel catalyst supported on ceria-alumina exhibits slightly higher
conversion values of syngas. The biogas reforming reaction catalyzed
by nickel-alumina doped with ceria catalyst seems to be an appropriate
process in order to produce syngas [10]. Various methods are available
for converting biogas into hydrogen fuel. A good example is, a GAPCR
(Gliding Arc Plasma Catalyst Reformer) which converts biogas into the

⁎
Corresponding author.
E-mail address: nlpanwar@rediffmail.com (N.L. Panwar).

http://dx.doi.org/10.1016/j.rser.2017.01.167
Received 11 September 2016; Accepted 28 January 2017
Available online 08 February 2017
1364-0321/ © 2017 Published by Elsevier Ltd.
R. Kadam, N.L. Panwar Renewable and Sustainable Energy Reviews 73 (2017) 892–903

Fig. 1. Route map of biogas conversion to transportation fuels adapted from [15].

higher percentage of hydrogen. At optimum conditions, H2 yield was Table 1

59%, energy efficiency and energy requirement were 53% and 289 KJ/ Composition of biogas and natural gas adapted from [17,18].
mole respectively [11]. The partial oxidation of methane by oxygen
Component Biogas Natural Gas
giving synthesis gas can be catalyzed to thermodynamic equilibrium
using transition metals. The yield of CO and H2 is increases with Methane (%) 40–75 87–97
atmospheric pressure [12]. The two processes Fischer-Tropsch synth- Carbon dioxide (%) 25–55 0.1–1.0
Hydrogen sulfide (ppm) 50–5000 NA
esis (FTS) and methanol to gasoline conversion (MTG) are widely
Ammonia (%) 0–1 NA
studied for upgradation. Fig. 1 provides a route map of biogas Water (%) 0–10 NA
conversion to transportation fuels. Nitrogen (%) 0–5 0.2–5.5
The main constituents of biogas are methane (CH4) and carbon Oxygen (%) 0–2 0.01–0.1
dioxide (CO2), but there are significant quantities of undesirable Hydrogen (%) 0–1 Trace−0.02

contaminants such as hydrogen sulfide (H2S), ammonia (NH3) and

siloxanes. The presence of these impurities is mainly depended upon
organisms within a landfill [20]. Many developed countries have
the biogas source, i.e. fermentation of manure. These can be detri-
targeted landfill methane recovery among greenhouse gas mitigation
mental to any thermal conversion device that may be corrosion, fouling
strategies since methane is second most important greenhouse gas
and harmful environmental emissions [13]. There are various methods
after carbon dioxide [21]. It is found that the mercury bearing
are available for biogas cleaning such as physical absorption, chemical
materials serve as bio reactors for the production of methylated
absorption, membrane separation, cryogenic separation and chemical
mercury compounds when they are placed in landfills. The mercury
conversion methods [14], and they are having capacity remove each
can be used from wide variety of resources such as fluorescent lights,
and all impurities, which are harmful to the thermal conversion
batteries, electrical switches, thermometers and general waste [22].
devices.
Before biogas is used as combustion fuel the hydrogen sulfide
The aim of this review paper is to cover various biogas purification
should be removed from the biogas. Some of contaminants in biogas
technologies, which are widely used all over the world. The working
such as hydrogen sulfide and water can cause maintenance issues.
and operation, merits and demerits, and the future scope of globally
When H2S is combusted in a boiler or CHP it can result in chemical
accepted biogas up-gradation technology have also discussed in this
corrosion [23]. It is also important to remove the water before using
review paper.
the biogas, slugs of water can damage gas compressors for example it
can also reduce the efficiency of CHP engines. Table 2 provides
2. Biogas cleaning requirement to remove impurities depending on utilization of biogas.
To upgrade biogas as biomethane the raw biogas should contain
Biogas production depends on type of feed material used, climatic more than 95% CH4 (with remainder as CO2), also biomethane can
conditions, production site and type of technology adapted for produc- directly injected into natural gas supply pipelines under suitable
tion. All these parameters affect the composition of generated biogas. circumstances [24]. Bureau of Indian standards also prescribed some
The main constituents of biogas are methane (CH4) and carbon dioxide standards to upgrade biogas as biomethane which are tabulated in
(CO2) along with some traces of gases such as water vapor, hydrogen following Table 3.
sulfide (H2S), nitrogen, hydrogen and oxygen [16]. Carbon dioxide and However biogas upgradation technique is followed on small scale.
traces gases must be removed because the hydrogen gas is corrosive Till 2013, the numbers of biogas upgrading plants in world were 250
and water vapor may cause corrosion when combined with H2S on and only 15 of them are in India [26]. Biogas is also converted into
metal surfaces and reduces the heating value. The composition of
biogas and natural gas is tabulated in following Table 1.
The biogas produced from anaerobic digesters contains 40–75% Table 2
methane while that of natural gas is 87–97% which is much higher Requirements to remove impurities depending on biogas utilization [23].
than biogas. The CO2 content of biogas is 25–55% and that of natural
Application H2S CO2 H2O Siloxanes
gas is 0.1–1.0% (Table 1). Biogas also contains traces of ammonia,
hydrogen sulfide, nitrogen, hydrogen and oxygen as compared to Boiler < 1000 ppm No No No
natural gas. Besides that landfill gas contains roughly 50–55% methane Cooker Yes No No No
Stationary engine < 250 ppm No No Yes
and 45–50% carbon dioxide with less than 1% non methane organic
Vehicle fuel Yes Recommended Yes No
compounds and trace amount of inorganic compounds [19]. Landfill Natural gas grid Yes Yes Yes Eventually
gas is a complex mixture of different gases created by action of micro-

893
R. Kadam, N.L. Panwar
Table 3
Requirements for biogas (biomethane) adapted from [25].
Characteristic Requirement
CH4, % 90
Moisture, mg/m3 16
H2S, mg/m3 30.3
CO2+N2+O2, % 10
CO2, % 4 99.1% and halogenated compounds by 99.9% [35]. The system was
O2, % 0.5
syngas by dry and auto thermal reforming that converts both CH4 and
CO2 into H2 and CO or syngas [27]. It is a valuable product that can be
used to produce liquid fuels, provides H2 for fuel cell and also improves
combustion of biogas.
There is various biogas purification methods are available such as
water scrubbing, chemical absorption, pressure swing absorption,
membrane separation and biofilters [28].
Purified biogas having advantages that it can reduce GHG emis-
sions as well as it having other environmental benefits. The water
scrubbing is commonly followed method for biogas purification.
Germany is global leader as well as market producer for biogas, till
2012 the functional biogas plants were 7470 including 80 biomethane
producing plant. Sweden is world leader in upgrading biogas to use as
transportation fuel. Till 2012, there were 47 biogas upgrading plants in
Sweden and increased by 22% since 2008 [29]. Countries like United
States, China, and India are in race to increase biogas upgradation
plants.
2.1. Pressurized water scrubbing
Pressurized water scrubbing is most commonly followed for biogas
purification. The CO2 and H2S are easily soluble than CH4 and easy to
operate. There is huge potential for biogas to be used as viable
transport fuel like CNG by compressing it and filling into the cylinders.
Chemical absorption of CO2 and H2S can also be done by packed
column with aqueous solution [31]. The aqueous solution is effective in
reacting with CO2 in biogas and creates CH4 enriched fuel. A CO2
scrubbing and bottling technology has been developed at IIT Delhi
[32]. The developed system removed CO2 and H2S from the biogas and
then compressed up to 20 MPa pressure and filled in high pressure
steel cylinders. A schematic diagram of simple pressurized water
scrubbing is shown in Fig. 2.
The raw biogas is pressurized to 9–12 bars and introduced at
bottom of the scrubbing tower. As soon as raw biogas moves up CO2
and H2S get dissolved within liquid column. The enriched biogas is
collected at top and water within impurities leaves from bottom [34]. It
having distinct advantage that chemicals are not required during entire
process. The only disadvantage of the system is that lot of water
Fig. 2. Flow sheet for water scrubbing technology adapted from [33].
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Renewable and Sustainable Energy Reviews 73 (2017) 892–903
required even with regeneration.
Current study on pressurized water scrubbing focuses on low water
usage and high pressure application. A pilot scale project was devel-
oped to upgrade municipal solid waste landfill gas. The effect of
parameters such as pressure (20–25 bars), temperature (10–25 °C)
and water flow speed (5.5–11 lit/min) were studied. The absorbent
water pH was between 4.4 and 4.9. The system reduced siloxanes by
operated at high pressure and low pH of absorbent water.
2.2. Pressure swing adsorption
Pressure swing adsorption is a process by which gases species from
the mixture of gases can be separated. The adsorptive such as zeolites,
activated carbon, and molecular sieve plays crucial role in adsorption.
This method relies on high pressure, the higher pressure the more gas
is adsorbed [36]. This method can be adapted to separate gas mixture
because different gases tends to attracted to different solid surfaces.
The separation is based on differences in binding forces to the
adsorbent. The volatile components with low polarity such as non-
adsorbable and opposes molecule like N2, CO and CO2 [37]. Biogas
purification and upgrading by pressure swing adsorption was studied
with synthetic and natural zeolites [38]. It is found that clinoptilolite is
best material because it is suitable for both purification and upgrading.
The breakthrough capacity of clinoptilolite was twice as the adsorption
capacity of synthetic molecular sieves. The high adsorption capacity of
173.9 mg CO2/g clinoptilolite was found which helped adjusting of
CH4/CO2 ratio in the biogas. In addition to that clinoptilolite is
completely regenerable and stable through several adsorption-deso-
rption cycles which having low cost. The schematic diagram of pressure
swing absorption is shown in Fig. 3.
The raw biogas is compressed to a high pressure in compressors
and then fed into adsorption column which retains only CO2 but not
CH4. When column material gets completely saturated with carbon
dioxide the pressure is released and carbon dioxide gets desorbed. The
desorbed carbon dioxide can be led into off gas stream. To operate PSA
process continuously several columns are required which should open
close consequently. Pressure swing adsorption includes feeding pres-
sure, purging pressure, adsorbent, cycle time and column intercon-
nectedness as main characteristics [40]. This method is very flexible
and can absorb variety of impurities in gases [41]. Zeolites are highly
porous adsorbent and most commonly used in world because it also act
as molecular sieves [42]. By using this method we can get purified
biogas with methane content of around 97% [43]. This method is also
used to upgrade landfill gas [44]. Vacuum pressure swing adsorption
with kinetic adsorbent, carbon molecular sieve 3 K was used to
separate carbon dioxide and methane. The results indicated that purity
of methane was higher than 96%. It was observed that a temperature
inside column increases and allows more faster desorption of CO2.
R. Kadam, N.L. Panwar
Fig. 3. Process diagram of pressure swing adsorption for biogas cleaning adapted from [39].
Fig. 4. Flow diagram of amine based H2S and CO2 scrubber adapted from [50].
Magnesium based metal organic framework (MOF) also known as Mg-
MOF-74 was successfully synthesized, characterized and evaluated for
adsorption [45]. It was found that the adsorbent Mg-MOF-74 prepared
for this study has medium pore width of 10.2 A, and BET specific
surface area of 1174 m2/g, CO2 and CH4 adsorption capabilities were
8.61 mmol/g (37.8 wt%) and 1.05 mmol/g (1.7 wt%) respectively. The
most important is that both CO2 and CH4 adsorption capacities are
significantly higher than those of zeolite 13 X under similar conditions.
A new column arrangement was developed to improve the utilization of
the adsorbent in multi-column pressure swing adsorption process [46].
In this column, when most adsorbed gas breaks through one column
and exit of this column is connected through to a second column
(trimbed) where more heavy gas get adsorbed. The increase in
performance is directly related to mass transfer zone which is inside
the column. The results showed that the obtained biomethane is of high
purity of 98%. This method is second most popular after water
scrubbing.
2.3. Amine gas treating (Amine absorption)
Amine gas treating also known as amine scrubbing, gas sweetening
and acid gas removal refers to a group of processes that uses aqueous
solutions of various alkyl-amines (commonly referred to simply as
amines) to remove hydrogen sulfide (H2S) and carbon dioxide (CO2)
from gases. It is commonly used in refineries and also used in
petrochemical and natural processing plants [47]. Many different
amines are used in gas treating such as diethanolamine (DEA),
Monoethanolamine (MEA), Methyldiethanolamine (MDEA),
Diisopropanolamine (DIPA), and Aminoethoxyethanol (DGA). The
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Renewable and Sustainable Energy Reviews 73 (2017) 892–903
most commonly used amines are DEA, MEA and MDEA.
Alkanolamines are widely used as absorbents for CO2 capture. The
structure consists of primary, secondary and tertiary amines. The CO2
loading capacity of tertiary amine is higher than those of primary and
secondary amines where the loading capacity lies between 0.5 and
1.0 mol of CO2 per mole of amine [48]. The reactions are as follows.
RR’NH+CO2 – RR’NH+COO-—————————— (1)
RR’NH+COO- + RR’NH – RR’NCOO- (carbamate)
+ RR’NH+2————————— (2)
The overall reaction is
2RR’NH + CO2 – RR’NCOO- + RR’NH+2 ————————— (3)
RRNCOO-+ H2O – RR’NH + HCO3-——————————————————
(4)
It was reported that bubbling of biogas with 10% of aqueous
solution of mono-ethanolamine can reduce CO2% from 40 to 0.5–
1.0% by volume [49]. Flow diagram of amine absorption process is
shown in Fig. 4 [50].
It consists of an absorption column, desorption column and water
wash scrubber. At first raw biogas enters the absorption column where
amine solution removes H2S and CO2. Then the biogas passes through
water wash scrubber where amine traces are removed and the
saturated amine passes through desorption column where it is regen-
erated. Nowadays piperazine (PZ) which is a cyclic diamine is used as
the promoter for CO2 capture because of its rapid formation of
carbonate with CO2 [51]. The effect of process conditions on the rate
R. Kadam, N.L. Panwar
of thermal degradation of concentrated, aqueous piperazine was
investigated [52]. In an industrial system with a simple stripper losses
due to thermal degradation are 0.043 molPZ/molCO2 captured. While
in case of second stage losses due to flashes are 0.0086 molPZ/molCO2
captured. The kinetics of N-Nitrosopiperazine formation from nitrite
and piperazine in CO2 capture was studied [53]. Piperazine is an
efficient in CO2 capture but it can form N-Nitrosopiperazine (MNPZ).
The reaction of nitrite was studied in 0.1–5 mol/dm3 PZ with 0.001–
0.08 molCO2/mol PZ at 50–135 °C. The developed mechanism
involved protonation of carbamate species, nucleophilic attack, carba-
mic acid and formation of bicarbonate and MNPZ. Concentrated
aqueous piperazine was studied as amine solvent for carbon dioxide.
The CO2 absorption rate of aqueous PZ was more than double that of
7 m MEA and the amine volatility at 40 °C was 11–21 ppm [54].
Degradation of 12 different amines with CO2 was evaluated in 100 mL
stainless steel batch reactors for 15 days at 140 °C with 4 mol/kg amine
solution and CO2 pressure of 2 MPa [55]. The cost of this method also
evaluated and it was 0.28 € Nm3 of biogas with yield of 90% and purity
of 98% [56]. Amine based absorption for CO2 has been mainly studied
for the removal of CO2 from the flue gases and from the power plants
with considerable techno-economical evaluation [57–60]. The advan-
tages of amine absorption are complete removal of H2S, high efficiency
and high reaction rates as compared to water scrubbing and ability to
operate at low pressure [61,62]. The disadvantages are additional
chemical inputs needed and waste chemical treatment is also needed
with waste chemical treatment. Another one is that corrosion due to
water vapors if temperature is reduced.
2.4. Membrane permeation
Permeation is also known as imbuing is the penetration of permeate
such as liquid gas or vapors through solid. It is directly related to the
concentration gradient of the permeate i.e. materials intrinsic perme-
ability and mass diffusivity [63]. Membranes and membrane process
were first introduced as an analytical tool in chemical and biomedical
laboratories [64–66]. The impurities like CH4 and CO2 can be
separated from the biogas by using membranes. The flow chart of
biogas purification is shown in Fig. 5. The method works on the
principle of pressure difference between gases. The membranes which
are available for separation can be grouped in to two main types: high
and low pressure membranes [67]. High pressure CO2/CH4 separation
was studied using SAPO-34 membranes at feed pressure up to
3.1 MPa. The highest CO2 permeance was 2.14×10−7 mol (m2spa) [68].
The high pressure membrane separation process is normally
operated at pressure less than 20 bars and in some systems it is
operated at 8–10 bars [69]. In multistage process the biogas is
upgraded to CH4 content more than 96%. Carbon molecular sieve
(CMJ) hollow fiber membranes have been investigated for CO2/CH4
separation up to 1000 psia. The mechanical permeance of CMJ
membranes under high pressure was encouraging and relevant for
CO2 removal from natural gas [70]. In multistage membrane separa-
Fig. 5. Flow sheet for membrane biogas purification process adapted from [34].
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Renewable and Sustainable Energy Reviews 73 (2017) 892–903
tion, waste gases from the first stages are recycled within process to
enrich the CH4 content of the final gas output [71]. Low pressure
membrane systems works at pressure close atmosphere. It is found that
using capillary module with polyamide membranes it is possible to
achieve membrane enrichment in single module where as to prevent
CH4 losses the multistage or hybrid systems should be used [72]. A
highly effective CO2 selective polyvinyl amine / polyvinlyalcohol
membranes was investigated for biogas upgradation. The process with
four different membrane module configurations with or without recycle
were evaluated and it was found that 2 stage cascade with recycle
configuration was proven optimal among four processes [73]. Dense
and asymmetric metal organic framework (MOFs) containing mem-
branes were prepared for CO2/CH4 and CO2/N2 binary gas mixture
separations [74]. The filter material such as [Cu (BTC) 2], ZIF-8 and
MIC-53 (A1) was used with membranes to increase thermal and
mechanical stability. The highest 40% wt loading, deteriorated the
properties of membrane. Both dense and asymmetric membrane
showed improvement in CO2/CH4 and CO2/N2 selectivity and per-
meance. A multiscale membrane based gas separation system was
developed. However single stage gas membranes have low purity and to
achieve high recovery it is necessary to install multistage membrane
separation plant [75].
Permselective membranes were used for removal of CO2 and H2S,
ultrathin polymer membranes have been found extremely effective for
purification. Facilitated transport membranes in which reversible che-
mical reaction occurs is perfect for CO2 absorption. The permeation
rates were relatively low and less attractive for biogas purification [76].
Gas liquid adsorption is newly developed process that uses micro-porous
hydrophobic membranes. The CO2 and H2S get dissolved in liquid while
remained methane can be used [77]. The separation of CO2 from CH4 by
using gas liquid membrane contractor was studied with0.2 µm pore size
micro-porous PVDF hollow fibers. Pure water, aqueous NaOH, and
aqueous MEA were used. The results showed that CO2 flux was
enhanced by the increase in NaOH solution but temperature increase
resulted in decreasing the CO2 flux [78]. However the CH4 recovery was
very high. A water swollen thin film composite membrane was tested for
effective separation of carbon dioxide from methane. Vapor condensing
conditions get created due to hydrophilic reverse osmosis membrane.
The feed gas gets dissolved in selective layer except methane. The
methane recovery from this condition was 95% volume of methane [79].
A novel biogas upgrading plant that produces 100 m3 (STP/h of fully
fledged natural gas substitute from about 180 m3 (STP)/h of raw biogas
was installed in Austria [80]. The advantage of membrane permeation is
that the processing equipment is compact and it requires low main-
tenance and energy. The disadvantages of membrane separation are
relatively low CH4 yield and high membrane cost. Some membrane
having low cost but difficulty is with yield and purity as well as fouling of
membranes which requires replacement with new one [34]. Recently
mixed matrix membranes were developed which having function to
combine the advantages offered by inorganic and polymeric materials.
[81].
R. Kadam, N.L. Panwar
Fig. 6. Biofilter system adapted from [83].
2.5. Biofilters
Biofiltration is a pollution technique which uses living material to
capture biologically degradable pollutants. This biofilters are com-
monly used for processing waste water, capturing harmful chemicals
and capturing contaminants from air [82]. Now a day's biogas is also
purified by using biofilters, chemotropic bacterial species such as
Thiobacillus genus is well suited to biogas conditions [28]. Another
bacterium namely chlorobium limicola is capable of oxidizing H2S in
the presence light and CO2. Chemotropic thiobacteria can purify H2S in
both aerobic and anaerobic conditions. Some bacterium like
Thiobacillus novellus, Thiothrix nivea can grow heterotrophically or
autotrophically and they are having ability of using available organic
material as their carbon source. Fig. 6 shows biofilter reactors devel-
oped for removal of hydrogen sulfide by complete aerobic oxidation in
acidic biofiltration.
The above biofilter is made of PVC pipe having inside diameter of
4.6 cm and height of 60 cm. The above biofilter was tested with 1:4
biogas to air ratio, the system achieved 94.7%, 87.3% and 85.6% H2S
removal efficiency at retention time of 160, 80 and 40 respectively. The
above biofilter showed a maximum elimination capacity of 256.49 g/
m3/h [83]. A small scale biofilter was developed by Fischer M.E. This
biofilter was operated for 61 days; the average H2S removal rate was
98.1 ± 2.9 for 34 days. Loading test was performed with loading rate of
27.8–69.5H2S/m3h and the H2S removal rate was 98.1 ± 2.9 for 20
days [84]. A chemical, biological process was performed to remove high
concentration H2S and the results revealed that H2S removal efficiency
was 98% for 1500 ppm H2S [85]. In this method the micro-organism
strain as it is for longer duration. Phototropic fixed film reactors are
interesting concept to remove H2S from the biogas [86]. They possess
ability to operate for longer periods without requiring a biomass
separation step and to work under variable load conditions. A two
phase bioreactor consisting of absorption column and aerobic biofilter
was developed. As bioreactor operation continued the pH was de-
creased from 6.3 to 1.5 and at this condition the sulfur oxidizing
bacteria was in experiential growth condition. The H2S removal
efficiency was greater than 97% [87]. The strain of micro-organisms,
pH and H2S removal efficiency remained as it is during experiment.
A pilot scale chemical, biological process was operated for 365 days.
The system achieved H2S removal efficiency of 95% under robust
conditions and 28.3 kWh of power was produced from purified biogas
[88]. A biotrickling filter packed with polypropylene pall rings was
tested for its ability to remove H2S from biogas under anoxic condi-
tions. The results indicated that 99% of H2S was removed when
controlled nitrate feeding was used [89]. Zicari in 2003 developed
biofilter with on farm cow manure compost as an H2S adsorption
column. The H2S removal efficiency of biofilter was over 80% and
elimination capacities were recorded between 16 and 118 gH2S/m3
bed/h. But still it's not clear that sulfur removed from biogas was done
biologically, chemically or physically [90]. Considering all biogas
purification techniques this method is eco-friendly and cost effective
[91–93]. Biofiltration is proven to be efficient in removing sulfur from
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Renewable and Sustainable Energy Reviews 73 (2017) 892–903
diluted gas streams [94–97]. Limited number of literature is available
on removal of high concentration sulfur. Surprisingly two methods are
used to remove high concentration sulfur from biogas. First one is
thiopaq process (Paques, The Netherlands) and second one is Biopuric
process (Biothane USA) [98]. The first one uses a conventional caustic
scrubber and expanded bed bioreactor. The Biopuric process uses
combination of chemical scrubber with biological treatment. The
advantages of biological methods are low energy requirement, mild
conditions and elemental sulfur byproduct. The output sulfur product
can be reused to produce other chemicals [99,100]. This method is also
having some disadvantages such as additional nutrients are required to
grow bacteria, small amount of O2 and N2 left in final output of biogas.
The H2S removal efficiency depends on activity of bacteria, various
study showed that this method can be cost effective upto 40 t per day
[28].
3. Comparison between different biogas upgradation
technologies
The methods which are used for purification of biogas are compared
for their methane purity, consistency and methane losses. As far as
European Union is concerned the highest share goes to water scrub-
bing, followed by pressure swing adsorption and chemical absorption
[101]. The pressure swing adsorption and membrane technology offers
progressive research potential. Today technological developments had
led to cheaper and more efficient plants. The upgrading cost of
established techniques is dependent on specific technology but more
importantly on the plant [102]. The amount of energy required to
upgrade biogas to biomethane is a key consideration while selecting
purification methods. Lower the energetic requirement for upgrading
the more net energy available [103]. Table 4 shows comparison which
was made between different biogas purification methods on the basis of
different parameters.
The efficiency of particular method which is employed for purifica-
tion is mainly depends on methane purity. Eyler suggests that methane
loss within purification system should be less than 0.5% [103]. While
some of manufactures allows a certain percentage of methane to
remain in a waste gas [104]. Another factor which plays important
role in selecting biogas upgradation technology is cost and mainte-
nance. Table 5 shows technical availability and maintenance cost of
upgrading technologies.
Biogas upgrading is beneficial but still its market is very small. The
most preferable technology is water scrubbing with share of 40%
followed by pressure swing adsorption and chemical scrubbing in
Europe. The most energy demanding technologies are chemical scrub-
bing and physical absorption but water scrubbing requires less energy.
4. Newly developed technology for biogas upgradation
The traditional methods of biogas upgradation are pressurized
water scrubbing, pressure swing adsorption, amine absorption, mem-
brane permeation and biological methods [105–110]. However some
R. Kadam, N.L. Panwar Renewable and Sustainable Energy Reviews 73 (2017) 892–903

Table 4
Comparison between different biogas purification methods [30,102].

Parameter PSA Water scrubbing Organic physical scrubbing Chemical scrubbing

Pre-cleaning needed Yes No No Yes

Working pressure, bar 4–7 4–7 4–7 No pressure
Methane loss < 3%/6–10% < 1%/ < 2% 2–4% < 0.1%
Methane content in upgraded biogas > 96% > 97% > 96% > 99%
Electricity consumption, kWh/Nm3 0.25 < 0.25 0.24–0.33 < 0.15
Heat requirement, 0c No No 10–100% 50–100%
Controllability compared to nominal load +/− 10–15% 50–100% 10–100% 50–100%
References > 20 > 20 2 –

Table 5
Technical availability and maintenance cost of different biogas upgradation Technologies
[103].
Upgrading Technical Maintenance cost, €/yr
technology availability, %
PSA 94 56,000
Water scrubbing 96 15,000
Chemical (amine) 91 59,000
scrubbing
Physical absorption 96 39,000
Membrane separation 98 25,000
new technologies like cryogenic upgrading and in situ enrichment have
been developed and they are under study [102,111]. The detailed
information of each method is given below.
4.1. Cryogenic upgradation
The traditional methods of biogas are in the stage of continuous
modification on the other hand cryogenic technology has been devel-
oped to purify and for bottling of biogas. It makes use of distinct
boiling/sublimation points of different gases particularly for carbon
dioxide and methane [102]. For example the boiling point of methane
(CH4) is −160 °c and carbon dioxide (CO2) is −78 °c at atmospheric
pressure. When raw gas gets cooled under pressure each single
constituent of biogas condenses at different temperature and by this
way separation is achieved [34]. The whole process is usually carried at
very low temperature which is −100 °c and high pressure of 40 bars.
The raw biogas can be cooled to temperature at which carbon dioxide is
condensed and can be separated in liquid and solid fraction while that
of methane accumulates in gas phase [112]. The principle of cryogenic
separation is shown in Fig. 7.
In cryogenic separation the raw biogas is passed through first heat
exchanger which cools gas at −70 °c. In next stage the cooled biogas is
passed through series of compressors and heat exchangers which cools
gas at pressure of 40 bars. Finally the gas enters in distillation column
where CH4 is separated from other impurities such as H2S and CO2.
The CPB concept (cryogenic packed bed has been developed to capture
CO2 from flue gases and biogas treatment [113]. The developed
mechanism was operated under similar conditions i.e. at a temperature
of −100 °c and high pressure of 40 bars to separate CO2 and CH4.
Cryogenic separation of biogas was also carried out by plate heat
exchangers. The biogas was upgraded at −1020c and it contained less
than 1% CO2. A higher biogas pressure was resulted in CO2 desublima-
tion temperature. The amount of desublimated CO2 was between 10.1
and 31.09 g [114]. The cryogenic technology is technically very
demanding but connected with high methane contents ( > 99%) and
low methane losses ( < 1%). The electrical energy demand is very low
which is 5–10% and hence it is environmentally friendly technique
[115]. This technology is still under development however in some
countries it is commercial. The commercial suppliers of cryogenic
technology are Scandinavian GTS, Aerion technologies/Terracasatus
technology and Prometheus energy.
The main advantage of cryogenic technology is that methane
content of purified biogas is upto 99%. Another advantage is that no
gas or chemicals are required and also pure CO2 is received as a
byproduct. The disadvantage of the system is that it is necessary to use
many technological types of equipment such as compressors and heat
exchangers which makes it expensive. Operator may face operational
difficulties while working on this method of purification [103,112].
4.2. In Situ methane enrichment
Another method for biogas purification is in situ methane enrich-
ment. The flow diagram of methane enrichment is shown in Fig. 8.
In first stage sludge from digester goes to desorption column and
again comes back to digester. In desorption column carbon dioxide is
desorbed by pumping air through sludge. Continuous pumping of air
leads to methane enrichment in digester. It is possible to get biogas
which having methane content of 95% and loss of methane below 2%
[102]. In situ methane enrichment is achieved using desorption
process by using modest recirculation rates. It is predicted that system
is capable of giving biogas containing 94% methane and it could be
modified to achieve CO2 removal efficiency greater than 60% [116].
Another simple in situ technique was developed to separate CO2 and
CH4 from biogas by using their solubilities. The CH4 purity was found
more than 98% however leachate recycle rates and alkalinity affects the
resulting offgas methane contents [117]. On the other hand high
recycle rates leads pH of digester above 8 which results in volatile
fatty acid accumulation and CH4 production rates.
A pilot scale enrichment experiments was studied for selective
desorption of carbon dioxide from sewage sludge. An external bubble
column of 90 dm3 and 140 dm3 were constructed for desorption. The
CH4 yield was constant during process and it is found that oxygen is
not having negative impact on CH4 producing activity. However CH4
loss was maintained below 8% [118]. Another in situ enrichment
experiment was studied by modeling. The bubble column with dia-

Fig. 7. Schematic diagram of cryogenic separation process adapted from [112].

898
R. Kadam, N.L. Panwar
Fig. 8. Process diagram of methane enrichment process adapted from [102].
meter of 0.3 m and variable height upto 1.3 m was used for study. The
desorption rates achieved for carbon dioxide were ranged from 0.07 to
0.25 m3CO2/m3 sludge per day. The amount of methane desorbed per
amount of carbon dioxide desorbed increases with increasing liquid
flow rates and decreasing gas flow rates [119]. A seven year study was
carried out on methane fermentation of energy crops like Sorghum,
Napier gas, Corn and in situ enrichment of biogas produced from these
crops. The aim of initial study was to assess methane production with
variable loading rates. The loading rate upto 12 gVs Kg−1 day−1 resulted
in methane production rates upto 3.3 L Kg−1day−1. Continuous feeding
of corn at rate upto 18 g Vskg−1day−1 resulted in 5.4 L Kg−1day−1. The
biogas was enriched by in situ enrichment process; the methane
content of offgas was more than 90% [120]. Steady state performances
of bubble column for desorption of carbon dioxide and methane was
analyzed by modeling but the experiment results were unsatisfactory. It
is believed that main problem was in experimental uncertainties not in
model [121]. However this method is still under research in worldwide
but more emphasis is on enzyme immobilization, bioreactor me-
chanics, enzyme cloning and cloning technologies.
5. Bio-CNG
Compressed natural gas (CNG) can be used in place of Gasoline
(petrol), Diesel fuel and Propane/LPG. CNG may be found above all oil
deposits or may be collected from landfills or waste water treatment
plants. It can be made by compressing natural gas to less than 1%
volume of atmospheric pressure and stored in container at a pressure
of 20–25 MPa [122]. Biogas formed in biomethane digester can be
stored in gas holder or balloon then it is purified to remove impurities.
The purified biogas is compressed and filled into cylinders. The gas is
known as biomethane or Bio-CNG [123]. Fig. 9 shows simple process
for Bio-CNG production.
Vijay et.al [32] developed unit for biogas purification and bottling
into CNG cylinders. After purification the enriched biogas was com-
Fig. 9. – Simplified process flow chart of Bio-CNG.
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Renewable and Sustainable Energy Reviews 73 (2017) 892–903
pressed upto 20 MPa using three stage cylinders. The Bio-CNG was
tested for vehicular operation. Another study was examined to use
biomethane as a CNG for bus fleet. The emissions from engine were
compared with bus operated on diesel fuels. The results showed that
there was substantial decrease in emissions from Bio-CNG buses [124].
Under suitable modifications vehicle can be operated on Bio-CNG and
few countries in world having Bio-CNG fuelling stations. Austria also
has set up their first Bio-CNG fuel station in Margarethan/Moos [125].
The operational experience also showed excellent suitability of upgrad-
ing as well as compressing biogas to produce Bio-CNG. Considering
global warming threat of Bio-CNG generated from Cassava starch
waste water treatment plant was assessed in Thailand [126]. The
energy analysis showed net energy ratio was higher than one i.e. net
energy gain. As far as global warming potential is considered Bio-CNG
is way better than fossil fuels like CNG and gasoline. A case study which
was carried out in Ireland showed that oil replacement with bio-
methane would directly save € 500 million out of € 5.9 billion [127]. A
5.9 kW stationary diesel engine was converted to spark ignition engine
to operate on CNG, Bio-CNG and biogas generated from Jatropha and
Pongamia oil seed cakes [128]. The Bio-CNG showed similar engine
performance as compared to CNG in terms of brake horse power and
specific gas consumption. By compressing the biogas reduces storage
requirements, concentrates energy content and increases pressure level
required to overcome resistance to gas flow [129]. A case study was
carried out on feasibility of filling biogas into cylinders in Punjab,
India. The biogas generated from corporation area was 28 m3 which
was then purified, compressed and filled into cylinders. The gas was
sufficient to provide fuel for 85.000 people [130].
A project was undertaken to compress and store biogas generated
from kitchen waste. A foot lever compressor was designed and biogas
was compressed to 4 bars in 0.5 m3 tank [131]. Well to tank (wtT)
analysis of biomethane was carried out in Gothenburg (Sweden). The
emissions of biomethane (Bio-CNG) and liquefied biomethane (Bio-
LNG) were estimated at 21.5 [g CO2 e/MJbiocng] and 26.2 [g CO2 e/
R. Kadam, N.L. Panwar
MJbiocng]. In case of diesel the emissions were reduced by 60–67%, 43–
47% and 64% [132]. Critical modification or conversion of engines is
necessary requirement to use Bio-CNG for vehicular operation.
6. Applications of biogas technology
Biogas can be used for various energy utilizations depending on
biogas source utilized for production. It can be directly used for heat
production by direct combustion, electricity production by fuel cells or
micro-turbines, CHP generation or as vehicle fuel [133]. However low
calorific value (LCV) of biogas is one of the most important bottlenecks
of biogas conversion into chemical or thermal energy [134]. The
applications of biogas are as follows:
6.1. Direct combustion of biogas
Biogas which is produced from digesters is used for various
purposes. However on small scale it is used for cooking [135].
Normally the biogas which is used for household cooking varies from
30 to 45 m3 per month [136]. Whereas the annual LPG consumption of
rural household is 101.4 kg and urban household is 119.3 kg [137] in
case of India. The biogas which is left in digester which is also known as
surplus can be used for water and space heating [138]. Direct burning
of biogas is not possible in commercial burners hence it needs some
modifications [139–141] but it can be directly burned without scrub-
bing though its calorific value is low. The domestic cookers are
normally supply natural gas at a pressure of 20 mbars, however for
biogas the minimum supply pressure is 10 mbars [142]. A study was
carried on air fuel ratio requirement for biogas burners and it is
recommended that air fuel ratio must be higher than 4:1 [143]. A
biogas stove was developed for community cooking applications. The
gas consumption rating of the developed stove was 1 m3 (19 MJ/h)
[144]. As far as the efficiency of stove is concerned it is nearabout 55%
[145]. The efficiency of biogas was evaluated for boiling water, cooking
rice and beans. The efficiency of cooking was 20%, 56% and 53%
respectively [146].
6.2. Power generation
Many developed countries now utilizing biogas for combustion
purposes to convert it into electrical and mechanical energy in
controlled combustion system by a heat engine [147]. Biogas can be
used in single cylinder, direct injection, compression ignition engine
which is modified to operate under duel fuel cell condition to generate
electricity [148]. The study was conducted to assess the economic
feasibility of electricity generation from biogas. The electricity price
was fixed at 0.07 €/kWh with payback period of 5.5 years [149]. Two
strategies were evaluated to increase the operating range of biogas
fuelled HCCI engine for power generation. First is oxygen enrichment
of inducted charge and second is gasoline pilot port injection [150]. In
Germany the biogas fuelled power plants are increased by almost 20%,
from 1050 in 2001 to 6000 in 2010 [151]. The models which are used
to predict biogas generation are modified with their constants and it
was tested with Mexican landfill gas model version 2.0. It was predicted
that by using modified the electricity generation could reach 2.4 MW in
2019 [152]. A thermodynamic model was developed for power
generation from biogas based on grape promace. The results showed
that it is possible to achieve 93.784 kWh per 1000 t of grape crushed
and it can cover 45% energy requirement of winery [153]. Biogas has
potential to generate electricity on demand. The demand driven biogas
production is vital for balancing power generation [154]. This technol-
ogy is still rare in most developing countries but in industrialized
countries like Germany this technology has become standard technol-
ogy.
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Renewable and Sustainable Energy Reviews 73 (2017) 892–903
6.3. Direct gas grid injection
To inject biogas into natural gas grid there are lot of legal, technical,
commercial and regulatory issues that needed to be considered. After
removing the impurities such as H2S and water vapor it can be injected
in natural gas grid network. Using the gas in an efficient modern
domestic boiler and transporting it through gas line system it can be as
efficient as 90% [155]. Another alternative to inject biogas into grid is
centralized injection facilities. By using this technology overall capital
and operating cost would be lower per unit of gas processed [156].
Energy efficiency evaluation of various biogas production and utiliza-
tion pathways showed that potential of primary energy input can be
increased upto 100% [157]. The influencing parameters to inject biogas
into natural gas grid are biogas composition, production capacity, gas
grid supply data and regional circumstances [158]. A model was
studied to explain green gas production also known as biomethane
by compressing several digesters. The results showed that there is no
single advantage of using a biogas digesters and centralized green gas
production by single large scale digester [159]. A case study on
greenhouse gas, energy assessment and injection into natural gas grid
showed that biogas which is produced from food industry waste and
manure can reduce greenhouse gas emission by approximately 90%
[160]. This technology is suitable alternative for the use of renewable
energy as compared to other technologies but new invention is
necessary to increase energy efficiency and benefits.
7. Perspectives of biogas technology
Biogas is combustible gas which mainly consists of methane (CH4)
and carbon dioxide (CO2) is produced by anaerobic digestion of organic
compounds. The methane is main constituent of biogas, it having
distinct feature that it can burn colorless, odorless. The biogas is
mainly used for cooking purposes but it also having capability to use as
transportation fuel for vehicles, electricity generation, combine heat
and power generation.
Before biogas to be used as transportation fuel or other purposes it
should be cleaned i.e. the impurities like H2S and water vapors should
be removed from the biogas. There are various methods are used for
biogas upgradation are water scrubbing, pressure swing adsorption,
membrane separation. Amongst them water scrubbing and pressure
swing adsorption are commonly followed. Nowadays biogas is directly
injected into methane gas grid which directly delivers gas to customers.
The biogas can be used for onsite electricity generation. One sewage
treatment plant in UK produces around 14,000 m3/day and this gas is
used in dual fuel engines of 520 kW. For a mixture of 67% CH4 and
33% CO2 specific power output can be 79% for air and compression
ratio of 15:1 [161]. A 5 hp engine can produce 4.14 kW by consuming
0.099 g/h/bhp diesel and 0.540 cum/bhp/h biogas which saves 70%
diesel. Therefore it is convenient to use duel fuel engine rather than
biogas engine. Biogas can be concentrated and compressed into
cylinders for vehicular operation. In Sweden trains and buses are
operated on biogas with refueling stations on streets. Biogas can be
compressed upto 120–150 kg/cm3 pressure to operate 95 bhp, 6
cylinders truck. By this it can travel 96 km distance in two stage
pressure reduction process [162]. Though it having certain limitations
such as water vapor and hydrogen sulfide can corrodes parts of engine
and also continuous adjustment of valve seat and tappet clearance. The
digester gas is also used for steam rising and direct heating. The
efficiency of coal fired boiler can increase by 10% by burning methane
[161]. The future of biogas is mainly focusing on feedstock, guidelines
to purify biogas to pipeline quality. The future of biogas will depend on
how markets of renewable energy will develop. The future there will be
lot of vehicles in world which will run on biogas or biomethane also
known as renewable natural gas.
R. Kadam, N.L. Panwar
8. Conclusions
Biogas is considered as major energy carriers in this modern era.
The gas can directly be used for space heating, generating thermal
energy, and electricity generation. The raw biogas have undesirable
impurities such as carbon dioxide and hydrogen sulfide. These
impurities can be removed to make it clean biomethane. The clean
biomethane can be compressed to increase the utility. Compressed
biomethane is called bio compressed natural gas (Bio-CNG) and can
directly be fed to transportation vehicles. The cleaning and up-grading
technologies which are commercially available in the market are water
scrubbing, pressure swing adsorption, and amine scrubbing. Advanced
cleaning and up-gradation technologies have already been entered into
commercial marked but yet not popularized. The technological im-
provements along with economical consideration are likely to be
continue in future as increasing fossil fuel prices. It is expected that
in the future, a harmonized biogas cleaning and up-grading methods
will be developed along with regulation for its utilization in different
applications.
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