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Treatment of cosmetic wastewater by a full-scale membrane bioreactor (MBR)

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Treatment of cosmetic wastewater by a full-
scale membrane bioreactor (MBR)

Victor M. Monsalvo, Jesus Lopez, Angel

F. Mohedano & Juan J. Rodriguez

Environmental Science and Pollution

Research

ISSN 0944-1344

Environ Sci Pollut Res

DOI 10.1007/s11356-014-3208-x

1 23
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 Author's personal copy
Environ Sci Pollut Res
DOI 10.1007/s11356-014-3208-x
RESEARCH ARTICLE
Treatment of cosmetic wastewater by a full-scale membrane
bioreactor (MBR)
Victor M. Monsalvo & Jesus Lopez & Angel F. Mohedano &
Juan J. Rodriguez
Received: 11 February 2014 / Accepted: 13 June 2014
# Springer-Verlag Berlin Heidelberg 2014
Abstract This work evaluates the treatment of wastewater
from a personal care products factory by a full-scale side-
stream membrane bioreactor (MBR) intermittently fed. The
wastewater contained particulate and soluble chemical oxygen
demand (COD) which is partially removed by physicochem-
ical pretreatment. Steady removal efficiencies above 98 %
were achieved for BOD5, COD and suspended solids. Fats,
oils and grease present in the raw wastewater were also
successfully removed. The MBR was operated at an average
permeate flux of 12 L/m2·h (LMH) working at a transmem-
brane pressure of 272±97 mbar. The soluble microbial prod-
ucts concentration remained fairly stable at 175±25 and 85±
15 mg/L for proteins and carbohydrates, respectively. This
maintained the filtration characteristics of the mixed liquor
unaltered over a long-term basis, which was evidenced by a
constant permeability of 43±19 LMH/bar. Most of the trace
organics detected in the wastewater were completely removed
and only some fragrances were detected in the permeate at
trace concentrations.
Keywords Cosmetic wastewater . Membrane bioreactor .
Personal care products . Water reuse . Revamping
Responsible editor: Bingcai Pan
V. M. Monsalvo (*) : J. Lopez : A. F. Mohedano : J. J. Rodriguez
Chemical Engineering Section, Universidad Autonoma de Madrid,
Francisco Tomas y Valiente 7, Madrid 28049, Spain
e-mail: victor.monsalvo@uam.es
J. Lopez
e-mail: jesusl.rodriguez@uam.es
A. F. Mohedano
e-mail: angelf.mohedano@uam.es
J. J. Rodriguez
e-mail: juanjo.rodriguez@uam.es
Introduction
Wastewaters from the manufacture of cosmetics are
characterised by relatively high values of chemical oxygen
demand (COD) of around 35 g/L, suspended solids (8 g/L),
and fats, oils and detergents (2 g/L) (Perdigón-Melón et al.
2010; Puyol et al. 2011). The main difficulty in treating
cosmetic wastewaters are the presence of detergents, surfac-
tants, personal care products (PPCP), pharmaceutical com-
pounds, preservatives (normally phenol derivatives), dyes,
fragrances and co-solvents, which are often nonbiodegradable
and/or toxic to microorganisms in biological systems
(Stackelberg et al. 2004, Aboulhassan et al. 2006, Bautista
et al. 2007). These effluents have been commonly treated by
means of coagulation and flocculation (Meiners 1994;
Moggio 2000). However, the increasingly stringent require-
ments concerning industrial wastewater treatment and reuse
demand the implementation of new or improved cost-effective
technologies. In this sense, the application of activated carbon
adsorption (Catalán Lafuente et al. 1974), ultrafiltration
(Huisman 2004), and advanced oxidation processes
(Bautista et al. 2007, 2010a, b; Naumczyk et al. 2013) has
been reported in the last years. The variable composition and
fluctuations in pollutant concentrations often make their treat-
ment by conventional activated sludge inefficient. Despite
this, the biological treatment of these effluents has scarcely
been studied. Anaerobic treatment in an upflow anaerobic
sludge blanket (UASB) reactor enabled COD removal effi-
ciencies close to 95 % (Puyol et al. 2011). However, this
wastewater showed a low methanogenic potential due to the
presence of inhibiting toxic species. This fact has been
claimed as the main limitation of industrial wastewater treat-
ment by anaerobic digestion (Skouteris et al. 2012). Aerobic
treatment in a sequencing batch reactors (SBR) has been also
tested. Total organic carbon (TOC) and COD reductions of 67
and 74 %, respectively, were achieved with a sequence
 Author's personal copy
including a 1-h anoxic stage at the beginning and the end of
each cycle. Additionally, nutrients were removed satisfactorily
by including anoxic stages along each cycle, allowing nitro-
gen and phosphorous removal above 97 and 70 %, respec-
tively (Tobajas et al. 2014).
One of the most crucial and difficult-to-control issue in
SBR is the separation of biosolids from the liquid phase. The
occurrence of sludge settleability problems in conventional
activated sludge-based systems, and poor clarification can
impede the re-use of the resulting effluent because of the
presence of high concentration of organic matter, solids and
pathogens. Therefore, conventional settling can be replaced
by membranes giving rise to membrane bioreactors (MBR).
This is currently a well-established technology for the treat-
ment of industrial wastewaters with increasing potential for
future applications. The microfiltration membranes of the
MBR system provide a barrier for bacteria, and in the case
of ultrafiltration (UF) also for viruses, thereby allowing a high
level of physical disinfection. A number of MBR plants are
currently operating in most Western European countries but
the resulting effluents are still barely being reused in spite of
their good quality (Melin et al. 2006). MBR is an efficient
treatment and the resulting effluent can be used for food crop
irrigation, landscape and golf course watering, vehicle wash-
ing, unrestricted recreational impoundment, toilet flushing
and industrial process water (Bérubé, 2010). The expectations
of customers, government regulators, and the public percep-
tion of the performance of MBR are likely to increase. The
study of cases where MBRs are used for water recycling
plants revamping will reinforce its application.
This work describes the application of a MBR for the
treatment of wastewater from a PPCP factory located near
Madrid (Spain). The current method of treatment consists of
homogenization, coagulation, neutralisation, flocculation, flo-
tation and biological oxidation in a SBR. Owing to revamping
and modifications of the piping, cleaning systems and process
units, the organic load of the wastewater has increased dra-
matically. This has caused a significant decrease in the perfor-
mance of the plant. On the other hand, increasing water needs
have promoted a new policy aimed at water reuse for general
purposes such as irrigation, hosing down, industrial car wash-
ing centres and fire extinguisher systems. In this context, and
taking into consideration land restrictions, the potential imple-
mentation of a MBR has been evaluated in this study.
Materials and methods
Design and operation of the wastewater treatment plant
The biological system consists mainly of an MBR. The fil-
tered water in the MBR is conducted to a permeate tank from
which the fluid returns to the membranes for back-flux
Environ Sci Pollut Res
cleaning. Two other tanks contain acid citric and sodium
hypochlorite solutions which are pumped to the membranes
during chemical cleaning. Two large blowers supply the mem-
brane modules with enough air to prevent fouling.
The UF membrane system used for the revamped plant was
designed to allow high flexibility because there is a wide range
of wastewater flow rates which can vary between 70 and
360 m3/day. The system uses a modular design which enables
any part of the plant to be revamped easily. The effluent from
the plant must be of proven quality for internal reuse. Online
monitoring and long-term logging of the water quality ensure
a reliable operation and water quality. Additionally, wastewa-
ter generation, energy consumption and the use of chemicals
have to be minimised.
Raw wastewater is homogenized in underground sealed
storage tanks. Under regular continuous flow conditions, the
quarry pool levels will fluctuate and so withdrawal from each
tank is automatically controlled. The full treatment setup
includes pre-treatment with coagulation, neutralisation and
flocculation units using polychlorinated aluminium as the
coagulant, sodium hydroxide to neutralise and a cationic
flocculant. The doses of coagulant and flocculant were
adjusted according to the jar tests following the protocol of
Krasner and Amy (1995). Under automatic control, the floc-
culant feed is regulated to guarantee rapid and optimum
flocculation. The flocs are separated in a dissolved air flotation
tank. This is followed by biological treatment in a stainless
steel tank where the dissolved oxygen concentration is main-
tained within 1–5 mg/L. The old air diffusion system was
designed for the previous SBR, which was run at a maximum
of 4,500 mg/L mixed liquor suspended solids (MLSS). Owing
to the higher MLSS concentration in the MBR (8–10 g/L),
prior to revamping the biological reactor was equipped with a
more powerful aeration system comprising two blowers and
membrane diffusers capable of providing 1,000 Nm3/h air
flow rate.
The quantity of nutrients in the raw wastewater was insuf-
ficient and consequently an external source (urea and phos-
phoric acid) was needed to achieve a COD:N:P ratio of
100:5:1. This ensured that the biological processes were not
limited by a lack of nutrients. The MLSS in the bioreactor was
maintained at between 8 and 10 g/L. The activated sludge is
recycled by pumping it from the membranes tank into the
bioreactor from where it overflows back to the membranes
tank. The biological tank was intermittently fed with pre-
treated (coagulation-flocculation) cosmetic wastewater every
8 h, operating at a hydraulic and sludge retention time of 2.5
and 17 days, respectively. Prior to entering the membrane
tank, the incoming pre-treated wastewater is passed through
a fine rotary screening filter (1.5 mm). A flow diagram of the
MBR system is depicted in Fig. 1 and the operating conditions
are summarised in Table 1. The MBR was operated for a
period of 2 years and several physicochemical parameters
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Environ Sci Pollut Res

Fig. 1 Flow diagram of the

membrane implemented
biological system

(see “Removal of trace organic compounds” section) were ventilation valves are opened and the permeate
followed in the inlet and exit streams. pump generates a high back flow.
The plant was fitted with two membrane modules im- Filtration The filtration valve is opened and the permeate
mersed in a single sidestream of 25 m3 tank, providing a total pumped from the membranes tank to the per-
filtration area of 1,000 m2. The mixed liquor is recycled from meate tank.
the biological tank to the membranes tank at a feed
flow/recycling flow ratio of approximately 1:4. A floatable
Table 1 Operating conditions of the MBR system
switch is also mounted in this tank to control the water level.
The average permeate flux through the membranes is main- Parameter Values Units
tained at 12 L/m2 h (LMH) and a filtration cycle of 5–6 min
Filtration flux 12 LMH
followed by a backflush of 30 s. A 30-s ventilation period is
Filtration time 300–360 s
set every 20 cycles with a weekly clean-up cycle, using 1 g/L
sodium hypochlorite and 2 g/L citric acid by a clean-in-place Backflush flow 30 LMH
(CIP) system which takes 90 min. The MBR was fitted with Backflush time 20–30 s
polyester sulfone (PES) UF hollow fibres (PURON®) 1.75 m Ventilation flow 6 LMH
length, 0.05 μm nominal pore size and an external diameter of Ventilation time 20–30 s
2.5 mm. The aeration system of the membranes tank was Ventilation frequency 20 cycles
divided into two sections providing two separate zones for Deaeration flow 25–30 m3/h
each membrane module which were aerated alternatively in Deaeration time 120 s
60-s cycles. The aeration time is 50 % of the filtration time. Deaeration frequency 4–6 h
Coarse bubble aeration is applied at a rate of 0.2 Nm3/m2 h, Maintenance cleaning 1 per week (168 h)
frequency
operating at a specific air demand of 23 Nm3/m3 permeate.
Maintenance cleaning 6 m3/h
Hollow fibres are degasified for 120 s every 6 h. Regular flow
flushing, together with the CIP procedures outlined in Table 1 Dosing pumps
enable the requisite steady-state flow rates to be maintained. OXI OXI 1,000 mg/L NaClO
The filtration sequence comprises the following stages: Dosing 1,800 s
Purging 600 s
Standby The system is maintained in standby if either the Air mix 300 s
level in the membranes tank is not sufficient, or Acid Acid 2,000 mg/L citric acid
any critical element fails. The module is aerated Dosing 1,800 s
and the other elements are switched off. Purging 600 s
Ventilation During this stage, the air entrapped in the air trap Air mix 300 s
is removed. This process is performed automat- Recirculation gravity IN min 4·feed
ically when the filtration sequence is started from Recirculation gravity OUT min 3·feed
standby. Permeate valves are closed and the
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Environ Sci Pollut Res

Backflush When the filtration time finishes, the permeate
pump changes the flow direction at a high rate
(30 LMH) for a specified time.
De-aeration After a defined number of cycles, the permeate
pump operates at a high flow in the filtration
direction to remove the air accumulated on top
of the hollow fibres.
Characterization of the wastewater
The main characteristics of the raw and pre-treated wastewater
are summarised in Table 2. As can be seen, the coagulation-
flocculation pre-treatment substantially reduces the COD
(85 %) and SS (84 %) of the raw wastewater. The amount of
fats, oils and grease also decrease significantly (86 %).
Analytical methods
COD, turbidity, total suspended solids (TSS) and volatile
suspended solids (VSS) were measured following the APHA
Standard Methods (APHA 2005). Protein and carbohydrate
concentrations were determined according to the adapted
methods of Lowry et al. (1951) and Dubois et al. (1956).
Bovine serum albumin (BSA) and d-glucose were used as
standards for the determination of protein and carbohydrate
content, respectively. Microbiological characterization was also
performed following the standard methods ISO 11731:1998
and UNE-EN ISO 9308–1 for Legionella sp. and Escherichia
coli. The identification of species in the wastewater and treated
effluents was performed by gas chromatography/ion trap mass
spectrometry and high-performance liquid chromatography/
refractive index (HPLC/RI). The GC/MS analyses were per-
formed in a CP-3800/Saturn 2200 Varian gas chromatograph
with an autosampler injector (CP-8200, Varian) and solid-phase
microextraction (carbowax/divinylbenzene, yellow green). A
Factor Four VF-5 ms capillary column (30 m length, 0.25 mm
diameter) was used as stationary phase. The flow rate of the
carrier gas (helium) in the GC/MS was 1 NmL/min. Sample
injection was carried out with splitless at 220 °C. The tempera-
ture program for the GC/MS analyses was ramped as follows:
40 °C for 15 min and 15 °C/min until 250 °C. The identifica-
tions were assessed with the aid of the database library NIST.
The removal efficiencies of trace organics was calculated by a
semi-quantitative approach considering the signals detected.
Organic acids and alcohols were quantified by HPLC/RI using
sulfonated polystyrene resin in the protonated form (67H type)
as the stationary phase (Varian Metacarb 67H 300–6.5 mm) and
sulphuric acid (0.25 mM in milliQ water) as the mobile phase at
a flow rate of 0.8 mL/min. The column temperature was 65 °C.
The images of the sludge flocs were obtained using the
bright field microscopic technique and a light optical micro-
scope (NIKON ECLIPSE Ci-S), equipped with a camera.
Scanning electron microscopy (SEM) images of the mixed
liquor were obtained using a Hitachi S-3000 N scanning
electron microscope. The image processing and analysis pro-
cedure comprised the image pre-treatment, segmentation and
debris elimination, whereas the image analysis program is
oriented to aggregates determination (Tian et al. 2011). The
image processing and analysis program for aggregates and
filamentous bacteria was developed in Matlab 7.6 (The
Mathworks, INC.) language. The first step of the procedure
consisted of the conversion of RGB images into grey-level
images and the subsequent background correction to reduce
the uneven background intensities caused by uneven lighting
from the image acquisition system. After the digital images
had been improved, the next step involved closing and thresh-
old segmentation in order to select the microbial flocs.
Results and discussions
Start-up and performance of the MBR
The quality of the effluent from the previous SBR system
regularly fulfilled the regionally established limits for

Table 2 Characteristics of raw and pre-treated cosmetic wastewater

Parameter Raw Pre-treated

pH 7.1±0.1
Conductivity (mS/cm) 0.9±0.1 1.6±0.8
COD (mg/L) 36,000±2,000 5,200±750
Soluble COD (mg/L) 23,600±1,300 4,500±950
BOD5 (mg/L) 7,200±500 1,100±200
TSS (mg/L) 8,000±700 1,300±300
VSS (mg/L) 5,600±500 900±200
Fat, oils and grease (mg/L) 1,700±300 234±86

Number of samples analyzed=12 Fig. 2 Time course of the SVI values in the previous SBR
 Author's personal copy
Environ Sci Pollut Res
Fig. 3 Time course of COD removal efficiency in the MBR
industrial wastewater discharge into the municipal sewer sys-
tem except for suspended solids. The occurrence of filamen-
tous bulking caused periodic dramatic fluctuations on the
settleability of the sludge giving rise to sludge volumetric
index (SVI) values up to 400 mL/g TSS (see Fig. 2).
The manufacturing policy of the PPCP plant has led in
recent months to increased volumes of high-strength wastewa-
ter. This resulted in a loss of around 10 % in the COD removal
efficiency of the existing SBR, reaching an efficiency of 86 %
when the organic loading rate (OLR) was increased up to 0.6 kg
COD/kg VSS·day. It is expected that further increases in the
OLR would cause a more severe drop in the SBR performance.
Fig. 4 GC/MS chromatogram of the raw cosmetic wastewater (see Table 3)
During the start-up of the MBR, a clear decrease in the COD
removal efficiency was observed, which appeared to be related
to the acclimation of the biomass to the new operating condi-
tions. After an acclimation period of 2 weeks, a noticeable
increase of the COD removal efficiency was observed, reaching
stable values close to 99 %. The discharge was characterised by
a biological oxygen demand (BOD5) of 13±5 mg/L, COD of
98±25 mg/L, conductivity of 2,600±700 μS/cm, and a con-
centration of fats, oils and grease of 10±5 mg/L. The presence
of suspended solids in the discharge from the previous SBR
was substantially decreased by the MBR, reaching concentra-
tions of 4±3 mg/L in the permeate. Thus, an average suspended
solids removal of 99 % was achieved.
The MBR effluents complied with the TSS Spanish limits
for water reuse (10–35 mg/L) for residential and urban uses.
Further increases in the removal of suspended solids would be
necessary to reach the limits recommended in some of the other
international guidelines (EPA 2004; Power 2010). The national
limits for water reclamation of turbidity (10 nephelometric
turbidity units, NTU), E. coli (200 colony-forming units per
litre, CFU/L) and Legionella sp. (100 CFU/L) were also ac-
complished. The resulting effluents were characterised by a
turbidity of lower than 1 NTU and undetectable levels of E.
coli and Legionella, which would permit a broad potential reuse
for general purposes such as irrigation, hosing down, industrial
car washing centres and fire extinguisher systems (Fig. 3).
 Author's personal copy
Environ Sci Pollut Res

Table 3 Assessment of the GC/MS peak in Fig. 4 and MBR removal concentration of some alcohols and organic acids such as glyc-
efficiencies
erol (100±3 mg/L), ethanol (30±2 mg/L), 2-propanol (4±1 mg/
Number Compound Removal efficiencya L), acetic acid (417±2 mg/L), formic acid (12.7±2 mg/L), and
(%) oxalic acid (1.1±0.2 mg/L).
The GC/MS signals observed in the analysis of the perme-
1 4-Hydroxi-bencenosulfonic acid 98.5
ate were 2 orders of magnitude lower than those detected in
2 3-Decanol >99.9
the fed wastewater. Therefore, most of the compounds had
3 2-Ethyl-1-hexanol >99.9
been completely removed and only some detected at trace
4 Benzyl alcohol >99.9
concentrations, reaching removal efficiencies of above 98 %
5 2-Methyl-6-metylene-2-octanol >99.9
in all cases. Some of the fragrances used in the formulation of
6 3,7-Dimethyl-1,6-octadien-3-ol >99.9
cosmetics were detected in the permeate at trace levels:
7 Phenylethyl alcohol >99.9 bicycle-4,10-hept-2-ene-3,7-dimethyl; 2-phenylethanol
8 Benzyl acetate >99.9 phenethyl (a floral odour); eucalyptol (a spicy aroma and
9 3,7-Dimethyl-1,6-nonadien-3-ol >99.9 taste); 1,6-octadien-3-ol-3,7-dimethyl synthetic linalool (a
10 1-Methanol-3-cyclohexen >99.9 thick green sweet wood green flavour); and 1-undecanol (a
11 1,5,5-Trimethyl-6-methylene- >99.9 citrus-like odour). The other trace organics detected were
cyclohexene
12 2-Phenoxyethanol >99.9
undecylenic acid (an antimicrobial used in cosmetics); benzo-
13 3,7-Dimethyl-2,6-octadiene-1-ol >99.9
phenone (which is used in bath products, nail polishes and
14 2,4-Diisocianate-1-methylbenzene 99.9
enamels, makeup products, hair products, sunscreens and skin
care products); 1-octanol (used in the synthesis of the esters
15 Methylparaben >99.9
present in perfumes and flavourings) and oleyl alcohol (a
16 Cyclododecane >99.9
thickener used in skin creams, lotions and many other cos-
17 3-Methyl-ciclopentyl-benzene >99.9
metic products). Several works have been published compar-
18 Ethylparaben >99.9
ing conventional activated sludge units and MBRs for the
19 Diethyl-phtalate >99.9
removal of a wide range of PPCP from wastewater, some of
20 Methyl p-tert-butylphenylacetate 98.3
which have shown that the MBR is a more efficient method
21 Propylparaben >99.9
(Le-Minh et al. 2010; Lyko et al. 2005; Coleman et al. 2009;
22 Methyl 3-oxo-2-pentylcyclopentane >99.9
acetate
Monsalvo et al. 2014). This has been attributed to the higher
23 Isobutylparaben >99.9 sludge retention time and the concentration of MLSS in the
24 Butylparabene >99.9 MBR, although it is widely accepted that both technologies
25 Dibutyl phtalate >99.9 have similar removal efficiencies when working under similar
conditions (Melin et al. 2006; Judd 2011; Tewari et al. 2010).
Number of samples analyzed=10
aWith respect to peak area Characteristics of the mixed liquor

Removal of trace organic compounds
Figure 4 depicts a representative GC/MS chromatogram of the
pre-treated cosmetic wastewater fed to the biological reactor.
The assessment of the peaks is collected in Table 3. The
HPLC/RI analyses enabled the quantification of the
The concentration of MLSS inside the MBR reactor remained
stable throughout the operation of the plant at an average and
maximum concentration of 8 and 10 g/L, respectively, with a
sludge production rate of 0.25 kg solids/kg COD. The oper-
ating conditions in the MBR caused fragmentation of the
flocs. Small, irregular and fragmented flocs, with a large

Fig. 5 SEM images (a) and size

distribution (b) of flocs from
MBR
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Environ Sci Pollut Res

quantity of dispersed bacteria were observed in the stationary

operation of the plant (Fig. 5a). A high concentration of free-
living bacteria was also commonly observed in the MBR due
to their complete retention by the membrane, and this often led
to an increase in the transmembrane pressure (TMP) (Arevalo
et al. 2009; Monsalvo et al. 2012). The size distribution of the
microbial flocs is shown in Fig. 5b, which is expressed in
terms of equivalent diameter of the projected area. The particle
characterization after 1 year of operation indicated an
unimodal distribution centred at a mean diameter of 26 μm.
During the start-up of the MBR, the concentration of
soluble microbial products (SMP) in the mixed liquor in-
creased by up to an average concentration of 175±25 and
85±15 mg/L for carbohydrates and proteins, respectively. The
density of filamentous bacteria also increased significantly
and occasionally they became dominant. According to the
previous study, the filamentous bacteria were found to have
serious negative effects on membrane permeability (Meng
et al. 2009).The mixed liquor purged from the MBR is
dewatered in a sludge thickener followed by a press filter
where both primary and secondary sludge are fed. The overall
sludge production is around 3,000 kg/day. A polymer dose of
0.57 kg/t of dry solids is added, giving rise to a final product
with a dry solids concentration of 30 % w/w, which is dis-
posed in a well-controlled landfill.
Membranes operation
Figure 6 shows the time course of the permeate flux, TMP and
mixed liquor permeability during one hour operation. The
average working flux was around 12 LMH at TMP of 272±
97 mbar. No significant fluctuations were observed in the
SMP concentration and the membrane permeability remained
in the range of 24–62 MH/bar. MBR is an efficient treatment
and the resulting effluent can be used for food crop irrigation,
landscape and golf course watering, vehicle washing,
Fig. 7 Time course of permeate flux (line) and TMP (squares) in the
MBR during long-term operation
unrestricted recreational impoundment, toilet flushing and
industrial process water (Bérubé, 2010).
As can be seen in Fig. 7, long-term operation of the MBR
under similar permeate fluxes led to constant TMP values which
suggests that the membranes were correctly cleaned using the
established protocol. Chemical cleaning solutions (Table 1) were
pumped from the CIP tank to the cell containing the membrane
modules. The membranes are in contact with the chemicals and
periodically aerated. The cleaning solutions were drawn from the
system at the completion of the cycle. During the recovery clean-
up, the membranes are submerged in the OXID solution for 6 h
and then in the citric acid solution overnight. After cleaning, the
membranes are rinsed and put back into service.
In some periods, the quantity of wastewater decreased
significantly as a result of lower production rates in the facto-
ry. During these times, the wastewater is stored in the under-
ground sealed storage tanks and an inlet flow is set. As soon as
this operation mode is activated, the wastewater inlet is
interrupted for 12 h and the wastewater fed every 24 h. The
air blowers in the biological reactor are switched-on and are
controlled by the PID depending on the dissolved oxygen
concentration and the set point established. The filtration
sequence is similar to that used under regular operation,
except that when the filtration is interrupted by the low level

Table 4 Operating costs of the MBR

Consumption Unit cost

(kg/m3) (€/kg)

Sodium hypochlorite 0.0325 0.22

Citric acid 0.0098 0.24
Sodium hydroxide 0.005 0.32
Urea 0.565 0.31
Phosphoric acid 0.061 0.54
Membranes replacement 0.30 1.76 €/m2
(m2/day)
Fig. 6 Time course of permeate flux (solid line), TMP (squares), and Electric energy (kWh/m3) 5.28 0.10 €/kWh
permeability (dashed line) in the MBR treating cosmetic wastewater
 Author's personal copy
alarm, the blowers in the membranes tank do not run contin-
uously, but follow programmed sequences.
In comparison with a conventional activated sludge sys-
tem, the MBR demands much more automation, not only for
start-up, but also for daily plant operation. Originally, the
permeate flow was controlled by the level in the aerobic
bioreactor, which caused instabilities in the filtering system.
The intermittent aeration gave rise to significant variations of
the level in the reactor as well as membrane flux fluctuations,
despite the influent flow remaining constant. Air accumula-
tion in the pipes which drive the sludge by gravity to the
membrane filtration trains, also posed some problems.
The system offers the common flexibility and performance of
a distributed control system (DCS) and is designed for the
minimum operator intervention whilst maintaining the necessary
interlocks for safe operation. To facilitate the control of the plant
a PLC-based system has been selected with a PC-based topology
incorporating a SCADA software package, for easy operation.
The visualisation system (man–machine interface) runs on PCs
connected to the PLC. The PC runs a software package and
represents the process configuration as MIMIC diagrams with
individual displays of plant items or equipment and faceplates
for control points. The combination of the visualisation and
MIMIC systems also offers trending, facilities, alarm handling,
operator prompts and messages, and data storage.
Cost analysis
The economic analysis summarised in Table 4 shows that the
consumption of chemical reagents which represents an important
component of the operating cost of the whole system (pre-
treatment and MBR) amounts to 0.87 €/m3. The energy cost
for pre-treatment, biological reactor and sludge treatment has
been estimated at 0.32 €/m3.
The costs of the MBR operation have been estimated,
assuming a membrane life of 5 years, and a wastewater
flowrate of 200 m3/day, for 24 h/day, for 240 day/year, on
average. The doses of sodium hypochlorite, citric acid and
sodium hydroxide were 32.5, 9.8 and 5.0 mg/L, respectively.
The electric power of the facility is 44 kW.
The cost of sludge treatment and disposal for both primary
and secondary sludge is 0.84 €/m3. The total operating cost of
the whole treatment plant is estimated at 3.3 €/m3, corre-
sponding to 1.27 €/m3 for the MBR and 1.19 €/m3 to the
pre-treatment. Thus, the operating costs of the wastewater
treatment plant with the SBR (2.6 €), before the plant
revamping, has increased slightly.
Conclusions
The full-scale MBR system showed a highly stable perfor-
mance for the treatment of wastewater from a personal care
Environ Sci Pollut Res
products factory. The resulting effluent fulfils the require-
ments for urban, agricultural and recreational reuse.
Although the mixed liquor exhibited poor permeability, the
membranes performance was fairly stable and the transmem-
brane pressure was maintained at constant values as a conse-
quence of the clean-up program. So far, the hydraulics of the
system has not failed, and the membranes removed practically
all the suspended solids. Despite the fact that chemical disin-
fectants are discharged into the treatment plant during clean-
up operations, the start-up of the biological reactor was ac-
complished in a short time because the biomass from the
former SBR system was used successfully in the new biolog-
ical reactor (MBR). Most of the trace organic compounds
identified in the cosmetic wastewater using GC/MS and
HPLC/RI analyses were not detected in the effluents from
the MBR after 30 days of operation. Furthermore, the effluent
complied with the Spanish criteria and most of the quality
specifications defined by the international guidelines and reg-
ulations for water reuse and reclamation.
Acknowledgments The authors greatly appreciate the financial support
provided by the Spanish MCI through project CTM2010-15682 and CTQ
2008–03988.
References
Aboulhassan MA, Souabi S, Yaacoubi A, Baudu M (2006) Removal of
surfactant from industrial wastewaters by coagulation flocculation
process. Int J Environ Sci Technol 3(4):327–332. doi:10.1007/
bf03325941
APHA (2005) Standard methods for the examination of water and waste-
water. none. APHA-AWWA-WEF, Washington, D.C
Arevalo J, Moreno B, Pérez J, Gómez M (2009) Applicability of the
sludge biotic index (SBI) for MBR activated sludge control. J
Hazard Mater 167(1):784–789. doi:10.1016/j.ejop.2011.06.001
Bautista P, Mohedano AF, Gilarranz MA, Casas JA, Rodriguez JJ (2007)
Application of Fenton oxidation to cosmetic wastewaters treatment.
J Hazard Mater 143(1–2):128–134. doi:10.1016/j.jhazmat.2006.09.
004
Bautista P, Mohedano AF, Casas JA, Zazo JA, Rodriguez JJ (2010a)
Oxidation of cosmetic wastewaters with H2O2 using a Fe/γ-Al2O3
catalyst. Water Sci Technol 61:1631–1636. doi:10.2166/wst.2010.
872
Bautista P, Mohedano AF, Menéndez N, Casas JA, Rodriguez JJ (2010b)
Catalytic wet peroxide oxidation of cosmetic wastewaters with Fe-
bearing catalysts. Catal Today 151(1–2):148–152. doi:10.1016/j.
cattod.2010.01.023
Bérubé, P. (2010) Sustainability science and engineering. Isabel, C.E. and
Andrea, I.S. (Eds), 255-292, Elsevier, New York.
Catalán Lafuente JG, Bustos A, Morá J, Cabo J (1974) Study of the
treatability of the waste water from a cosmetics factory. Doc Invest
Hidrol 18:271–284
Coleman HM, Troester M, Khan SJ, McDonald JA, Watkins G, Stuetz
RM (2009) Assessment of trace organic chemical removal by a
membrane bioreactor using gas chromatography/mass spectrometry
and a yeast screen bioassay. Environ Toxicol Chem 28(12):2537–
2545. doi:10.1897/08-531.1
 Author's personal copy
Environ Sci Pollut Res
Dubois M, Gilles KA, Hamilton JK, Rebers P, Smith F (1956)
Colorimetric method for determination of sugars and related sub-
stances. Anal Chem 28(3):350–356
EPA U (2004) Guidelines for water reuse EPA/624/R-04/108 Washington
DC, USA, 2004. Washington DC, USA.
Huisman I (2004) Optimising UF for wastewater treatment through
membrane autopsy and failure analysis. Filtr Separat 41(3):26–27.
doi:10.1016/S0015-1882(04)00146-6
Judd S (2011) The MBR book: principles and applications of membrane
bioreactors for water and wastewater treatment. Elsevier, New York
Krasner SW, Amy G (1995) Jar-test evaluations of enhanced coagulation.
J Amer Water Works Assn 87(10):93–107
Le-Minh N, Khan SJ, Drewes JE, Stuetz RM (2010) Fate of
antibiotics during municipal water recycling treatment pro-
cesses. Water Res 44(15):4295–4323. doi:10.1016/j.watres.
2010.06.020
Lowry O, Rosebrough N, Farr A, Randall R (1951) Protein measurement
with the Folin phenol reagent. J Biol Chem 193:265–275
Lyko S, Wintgens T, Melin T (2005) Estrogenic trace contami-
nants in wastewater-possibilities of membrane bioreactor
technology. Desalination 178(1):95–105. doi:10.1016/j.desal.
2004.12.016
Meiners H (1994) Purification of wastewater from cosmetic production.
Parfuemerie und Kosmetik 75:204–205
Melin T, Jefferson B, Bixio D, Thoeye C, De Wilde W, De Koning J, Van
der Graaf J, Wintgens T (2006) Membrane bioreactor technology for
wastewater treatment and reuse. Desalination 187(1):271–282. doi:
10.1016/j.desal.2005.04.086
Meng F, Chae S-R, Drews A, Kraume M, Shin H-S, Yang F (2009)
Recent advances in membrane bioreactors (MBRs): membrane
fouling and membrane material. Water Res 43(6):1489–1512. doi:
10.1016/j.watres.2008.12.044
Moggio G (2000) Pre-treatment implementation for industrial effluents
from a cosmetic industry. Tecnol. Chim. (3):60-64.
Monsalvo V, Shanmugam P, Horan N (2012) Application of microbial
indices to assess the performance of a sequencing batch reactor and
membrane bioreactor treating municipal wastewater. Environ
Technol 33(18):2143–2148. doi:10.1080/09593330.2012.660652
View publication stats
Monsalvo VM, McDonald JA, Khan SJ, Le-Clech P (2014) Removal of
trace organics by anaerobic membrane bioreactors. Water Res 49:
103–112. doi:10.1016/j.watres.2013.11.026
Naumczyk J, Bogacki J, Marcinowski P, Kowalik P (2013) Cosmetic
wastewater treatment by coagulation and advanced oxidation pro-
cesses. Environ Technol 35(5):541–548. doi:10.1080/09593330.
2013.808245
Perdigón-Melón JA, Carbajo JB, Petre AL, Rosal R, García-Calvo E
(2010) Coagulation-Fenton coupled treatment for ecotoxicity reduc-
tion in highly polluted industrial wastewater. J Hazard Mater 181(1–
3):127–132. doi:10.1016/j.jhazmat.2010.04.104
Power K (2010) Recycled water use in Australia: regulations, guidelines
and validation requirements for a national approach. National Water
Commission
Puyol D, Monsalvo VM, Mohedano AF, Sanz JL, Rodriguez JJ (2011)
Cosmetic wastewater treatment by upflow anaerobic sludge blanket
reactor. J Hazard Mat 185(2–3):1059–1065. doi:10.1016/j.jhazmat.
2010.10.014
Skouteris G, Hermosilla D, López P, Negro C, Blanco Á (2012) Anaerobic
membrane bioreactors for wastewater treatment: a review. Chem Eng J
198–199:138–148. doi:10.1016/j.cej.2012.05.070
Stackelberg PE, Furlong ET, Meyer MT, Zaugg SD, Henderson AK,
Reissman DB (2004) Persistence of pharmaceutical compounds
and other organic wastewater contaminants in a conventional
drinking-water-treatment plant. Sci Total Environ 329(1–3):99–
113. doi:10.1016/j.scitotenv.2004.03.015
Tewari PK, Singh RK, Batra VS, Balakrishnan M (2010) Membrane
bioreactor (MBR) for wastewater treatment: filtration performance
evaluation of low cost polymeric and ceramic membranes. Sep Purif
Technol 71(2):200–204. doi:10.1016/j.seppur.2009.11.022
Tian Y, Chen L, Zhang S, Cao C, Zhang S (2011) Correlating membrane
fouling with sludge characteristics in membrane bioreactors: an
especial interest in EPS and sludge morphology analysis. Biores
Technol 102(19):8820–8827. doi:10.1016/j.biortech.2011.07.010
Tobajas M, Polo AM, Monsalvo VM, Mohedano AF, Rodriguez JJ
(2014) Analysis of the operating conditions in the treatment of
cosmetic wastewater by sequencing batch reactors. Environ. Eng.
Manage. J. (in press).