Advances in Environmental Research 8 (2004) 455–466

Microfiltration of water-based paint effluents

B.K. Deya, M.A. Hashima, S. Hasanb, B. Sen Guptac,*
a
Institute of Post Graduate Studies and Research, University of Malaya, 50603 Kuala Lumpur, Malaysia
b
Department of Nuclear Engineering, University of Missouri-Columbia, Columbia, MO 65211, USA
c
School of Chemical Engineering, Queens’ University Belfast, Northern Ireland, BT9 5AG Belfast, UK

Received 5 September 2002; accepted 29 October 2002

Abstract

The major hurdle associated with water recycling in water-based paint manufacturing processes is microbial
contamination and related deterioration of product quality and shelf life. The common problems associated with
microbial degradation are change in viscosity, pH, colour and loss of surface adhesion properties. Owing to these
reasons, water recycling is not widely practised in water-based paint manufacturing processes. The present study
focuses on tertiary treatment of effluent by chemical coagulation and cross-flow microfiltration (0.2 mm pore size)
to produce water of sufficient quality for reuse in various stages of water-based paint manufacturing. The coagulation
and flocculation were carried out in a ‘jar test’ rig at a controlled pH, and coagulant dosage was optimised by
turbidity and zeta potential measurements. The filtrate was subjected to cross-flow microfiltration and permeate was
tested for necessary quality attributes. Screening of aerobic microbes and fungi were conducted by streaking the
samples on nutrient agar and malt extract agar, respectively. Iron sulfide agar tubes were used for screening anaerobic
microbes or the sulfate reducing bacteria. The tests showed that permeate was free from microorganisms. The process
was implemented in a paint manufacturing plant in Malaysia, which resulted in 55% reduction in water consumption.
䊚 2002 Elsevier Science Ltd. All rights reserved.

Keywords: Microfiltration; Water recycling; Microbial contamination; Water-based paint

1. Introduction is generated primarily due to cleaning operations of

Latex paints generally consist of organic and inorgan-
ic pigments and dyestuffs, extenders, cellulosic and non-
cellulosic thickeners, latexes, emulsifying agents, anti
foaming agents, preservatives, solvents and coalescing
agents. Due to the varying degree of chemicals used,
the wastewater contains appreciable concentrations of
BOD, chemical oxygen demand (COD), suspended
solids, toxic compounds and colour. The treatment of
latex paint wastewater for reuse thus requires effective
treatment for the removal of suspended solids, metal
ions and microorganisms.
In manufacturing paint and allied products, all the
constituents entering mixers or reactors come out as
products and, as such, there is no major stream of
wastewater associated with the production. Wastewater
*Corresponding author.
E-mail address: b.sengupta@qub.ac.uk (B. Sen Gupta).
mixers, reactors, blenders, packing machines and floors.
In general, paint effluents are alkaline and have high
BOD, COD, heavy metals, suspended solids and col-
oured materials (Dey, 1999). Recovery of water from
paint effluent is an attractive option as it substantially
reduces the fresh water consumption in the process.
Anderson et al. (1981) reported the use of reverse
osmosis for the treatment of paint wastewater for recy-
cling purposes. In this process, high quality feed water
was derived from the electrocoat painting bath by
reverse osmosis. Uenoyama et al. (1996) reported a
case study of successful recycling of water at a Nippon
Paint plant in Japan. In this case, the waste stream from
a water-based paint manufacturing process was used to
recover pigment, and water for cleaning purposes.
Microbiological spoilage of water-based surface coat-
ings can result in severe economic losses to the manu-
facturers and end users. The effects of bacterial and

1093-0191/04/$ - see front matter 䊚 2002 Elsevier Science Ltd. All rights reserved.
PII: S 1 0 9 3 - 0 1 9 1 Ž 0 2 . 0 0 1 2 2 - 3
456 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466
Table 1
Effects of microbial degradation on paint ingredients
Attack on cellulosic thickeners
Attack on dispersants
Attack on glycols, coalescing agents
Attack on antifoam
Attack on dispersed colour
fungal activity are viscosity loss, gassing, malodour and
visible surface growth. In addition, discoloration and
alteration in the rheology of the formulation can result
in the product being unacceptable to the customer. In
addition to these obvious problems, the presence of
microbially produced enzymes can lead to changes in
the product long after manufacture (Briggs, 1977; Dey,
1999).
Microorganisms thrive well in water-based paint.
They quickly consume the available oxygen allowing
anaerobic growth to commence. Both bacteria and fungi
are capable of producing cellulase, an enzyme remark-
ably effective at concentrations as low as 10y5 units
per cm3, at breaking down long chain cellulosic thick-
ening agents, producing small oligomeric residual units
which do not fulfil the function of the original material.
Fermentative bacteria would produce gas from break-
down of the cellulosic thickener degrading the cellulose
first to glucose, which is then fermented to yield acid
and carbon dioxide. In the presence of fillers such as
calcium carbonate, further gas can be produced by
action of the biogenic acids (Briggs, 1977; Dey, 1999).
Other bacteria known as sulphate reducers, for example
Desulphovibrio desulphuricans, under anaerobic condi-
tions can utilise oxygen from sulphates leading ulti-
mately to the formation of hydrogen sulphide.
Opperman and Goll (1984), in their study of contami-
nated emulsion paints, concluded that more than a
quarter were infected with these and other anaerobic
organisms. Such sulphate reducing bacteria (SRB) are
responsible for the most commonly noticed malodour
associated with emulsion paint spoilage. Formation of
insoluble sulphides such as iron sulphide can cause
discoloration. Other organisms such as Rhodotorula
rubra and Sporobolomyces roseus and pigmented mould
fungi can also produce discoloration. Acid production
by microorganisms can cause pH shifts although paints
are normally well buffered to withstand rapid spoilage.
A summary of effects of microbial degradation on paint
ingredients in a formulation is shown in Table 1 (Dey,
1999).
The present study focuses on the tertiary treatment of
effluent by enhanced chemical coagulation and cross-
flow microfiltration to produce water that is of sufficient
quality for reuse in various production stages. In this
study, the effluent from a modern paint manufacturing
Viscosity loss, gas production, pH shifts
Poor hiding, colour shifts, precipitation of pigments, gelling
Gloss reduction, poor freeze thaw stability, chalking, porous
film, poor adhesion, poor levelling
Foam, porous film
Off-colour, uneven colour, agglomeration of colorant
plant in Kuala Lumpur was used for this purpose. The
company could comply with the discharge regulations
set by Department of Environment (DOE), Malaysia.
However, the management was keen to reduce the
effluent volume and regenerate process water from the
effluent as far as possible. The company employed
physical and chemical treatment methods to treat was-
tewater generated from the production and cleaning
processes. The treatment plant consisted of an equalis-
ation basin, a primary settling tank, a flash mixing tank
(where sulphuric acid, lime, alum, polymers and bio-
nutrients are added for pH control and coagulation),
two aeration tanks, a secondary settling tank and two
holding tanks. Wastewater from the manufacturing plant
was conveyed by gravity flow to the treatment plant.
Here the colloidal particles or suspended solids in the
waste water, coloured materials, BOD, COD and heavy
metals were reduced to Standard B limits of the Malay-
sian Environmental Quality Act 1974 (Amendment
1996) prior to discharging to a public sewer system.
2. Materials and methods
2.1. Sampling procedures
Composite samples of effluent were collected from
two points, the equalisation tank and the effluent dis-
charge out fall. Twenty samples were collected from
each point. Sampling of the wastewater was carried out
according to Standard Methods for the Examination of
Waste Water (APHA, 1992).
2.2. Waste water characterisation
Effluents from the equalisation tank and the outfall
were completely characterised in this study. Moreover,
outfall samples were analysed after further treatment,
namely chemical coagulation and membrane filtration
following coagulation. All samples were analysed fol-
lowing the procedures outlined in the Standard Methods
(APHA, 1992).
2.3. Chemical coagulation and analysis
Laboratory scale evaluation of chemical coagulation
and flocculation was performed using a six-place jar
 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466
test apparatus equipped with multi-speed mixing stirrers.
The jar test procedure included high sheer mixing at
100 rpm for 5 min, followed by 30 min flocculation at
20 rpm and a 1 h of settling sequence. Experiments
were carried out with 300 ml of liquid, which was
equivalent to 4.8 cm of liquid in a jar. Supernatant was
withdrawn at a height of 1.6 cm from the top using a
hypodermic needle. At this depth, neither any floating
particle was sucked in nor the sludge was resuspended
due to suction. The suspended solids concentration (T)
was determined by turbidity meter (Jenway, UK Model
No. 6035). The relative turbidity, TyT0 where T0 is T in
the absence of chemical coagulants was employed in
order to assess the efficiency of the coagulant and
flocculant used. The inorganic chemicals like alum
(Fluka Chemicals, UK), calcium hydroxide (Ajax
Chemicals, Malaysia) and anionic polyelectrolyte
(Aldrich Chemicals, UK) used for flocculation were of
analar grade. Polyelectrolyte (anionic polyacrylamide)
was added to the sample as a freshly prepared, 0.25%
solution. Fresh polyelectrolyte solution was prepared
daily from a 3% stock solution.
First, the optimum pH for the function of alum and
lime was determined. Varying doses of polyelectrolyte
were then added at the optimum pH and alum dose.
Apart from this, mixing time, mixing speed, age of
polymer, and mixer geometry were held constant to
avoid the introduction of additional variables to the
system. The clarification efficiencies were measured in
terms of turbidity and COD. Once the optimum dosage
of alum and polyelectrolyte had been determined, larger
quantities of wastewater were treated and a full analysis
of parameters listed in Standard B of the Industrial
Effluent Regulation 1989 (Malaysia) were carried out.
All parameters were analysed according to procedures
outlined in Standard Methods (APHA, 1992).
2.4. Membrane filtration
A bench scale cross-flow microfiltration membrane
unit (Sartorius GmbH Model No. SM 16650) was
employed to accomplish further clarification and disin-
fection of the treated effluent for recycling purposes.
The set-up consisted of a feed tank, a pump with
adjustable speed and the filter equipment. The trial was
carried out utilising 0.01 m3 (10 l) of treated effluent
and permeate was collected in a measuring cylinder.
The cumulative volume of permeate was recorded at 15
s interval.
All the experiments were carried out using a cellulose
acetate flat sheet membrane (0.2 mm). It was cleaned
after each experiment in three stages using 0.1 N HCl,
followed by 0.1 N NaOH and 0.6% hydrogen peroxide.
The membrane was thoroughly cleaned with deionised
water after each stage to remove any reagent residues.
Pure water permeability tests were carried out to assess
457
the cleanliness of the membrane. The experimental set-
up is shown schematically in Fig. 1. A micro pump
(Micro-Tech Scientific, CA, USA) was used to achieve
a constant feed flow rate. The flow rates were monitored
using a Dwyer Rate—Master flow meter (Sherman
Instruments, NJ, USA). The pressure levels were adjust-
ed manually by in-line valves and by controlling the
speed (rpm) of the peristaltic pump. Compressed air
was used to maintain constant pressure in the feed tank
as well as to purge residual water after each cleaning
cycle. The operations were carried out at a transmem-
brane pressure drop of 0.3 bar and at a maximum cross-
flow velocity of 0.3 mys. All the operations were carried
out under total recycle mode, using a peristaltic pump
to return permeate to the feed tank and maintain the
consistency of the feed.
2.5. Microbial tests
The samples of effluent emanating from the waste-
water treatment plant (WWTP) as well as the effluent
subjected to additional treatments were subjected to
microbiological tests. The samples were collected in
sterilised bottles and stored at 4 8C prior to the test.
The pH and redox potential measurements were initially
recorded. The samples were then screened for microbi-
ological contamination. The growth of microorganisms
was assessed after 48 h incubation period. Total viable
counts were conducted for samples showing positive
results in the screening stage.
2.5.1. Screening for aerobic microbiological
contamination
Aliquots of each sample were inoculated by streaking
onto plates of nutrient and malt extract agars for the
detection of bacteria and fungi (including yeast), respec-
tively. After incubation for at least 48 h at 25 andyor
30 8C, the resulting microbiological growth was visually
assessed using a rating scale of 0–6 with 0 indicating
no growth and 6 indicating dense growth.
2.5.2. Screening for anaerobic sulphate reducing
bacteria
Each sample was streak inoculated into tubes of
sulphate iron media (SIM)yiron sulphate agar (ISA).
After incubation at 30 8C, the resultant growth of SRB
was visually assessed according to the degree of black
coloration developing.
2.5.3. Total viable count by miles and misra technique
(Miles and Misra, 1938)
Serial dilutions of each sample were prepared in
sterile 1y4 strength Ringer’s Solution. Duplicate 25 ml
drops of each dilution were pipetted onto the surface of
well-dried nutrient and malt extract agars for the detec-
tion of bacteria and fungi (including yeast), respectively.
458 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466

Fig. 1. Experimental set-up for the microfiltration of effluent.

After incubation at 25 andyor 30 8C for a minimum of
24 h (bacteria) and 48 h (moulds and yeast), the
numbers of colonies from a ‘countable’ drop were
recorded.
3. Results and discussion
3.1. Waste stream characterisation
The influent (untreated wastewater) and effluent ema-
nating from the plant’s wastewater treatment facility
were characterised and are shown in Tables 2 and 3,
respectively. In principle, the concentration of the efflu-
ent emanating from the WWTP should comply with the
limits proposed by the DOE, Malaysia. However, the
effluent did not meet the proposed effluent standards.
Under these circumstances, the management of the
company decided to subject the stream to further treat-
ment with the idea of recycling water. In this study,
major pollutants were analysed based on composite
samples collected from the main effluent channel.
3.2. Coagulation and flocculation studies
Numerous jar tests were carried out in order to
establish a practical understanding of the coagulation
performance for this application. Initially the tests were
carried out to determine the optimum pH for the
 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466 459

Table 2
Physico-chemical characteristics of the influent stream

Parameters Unit Minimum Maximum Averagea Std. Bb

pH 8.0 9.3 8.5 5.5–9.0
BOD5 @ 20 8C mgyl 450 598 588 50
COD mgyl 4500 5868 5632 100
TSS mgyl 2784 3824 2864 100
Temperature 8C 29.5 30.2 30.2 –
Turbidity NTU 4896 5854 5632 –
DO mgyl 0.05 0.79 0.58 –
Mercury as Hg mgyl 0.012 0.035 0.031 0.05
Cadmium as Cd mgyl ND(-0.003) ND(-0.003) ND(-0.003) 0.02
Hexa-chromium as Cr6q mgyl ND(-0.02) ND(-0.02) ND(-0.02) 0.05
Cyanide as CN mgyl ND(-0.02) ND(-0.02) ND(-0.02) 0.10
Lead as Pb mgyl ND(-0.02) 0.15 0.12 0.5
Tri-chromium as Cr3q mgyl 0.02 0.09 0.06 1.0
Copper as Cu mgyl ND(-0.003) 0.098 0.095 1.0
Manganese as Mn mgyl 0.048 0.065 0.057 1.0
Nickel as Ni mgyl 0.030 0.048 0.04 1.0
Tin as Sn mgyl ND(-0.01) ND(-0.01) ND(-0.01) 1.0
Zinc as Zn mgyl 0.154 0.198 0.173 1.0
Boron as B mgyl 1.3 1.9 1.7 4.0
Iron as Fe mgyl 0.42 0.58 0.48 5.0
Phenol mgyl 0.34 0.057 0.036 1.0
Free chlorine as Cl2 mgyl ND(-0.02) ND(-0.02) ND(-0.02) 2.0
Sulphide as S2y mgyl ND(-0.1) ND(-0.1) ND(-0.1) 0.5
Oil and grease mgyl ND(-2) ND(-2) ND(-2) 10.0
Untreated wastewater.
a
Average of 20 samples.
b
DOE (Malaysia) Std. B parameter limits for discharge of effluent to inland waters below water intake points.

function of alum. A fixed dose of alum was added to
the effluent wastewater and the pH of the mixture was
then adjusted with calcium hydroxide and sulphuric
acid. For jar test purposes, the effluent water was
suitably diluted with filtrate so that the zeta potential of
the system does not change due to dilution. The effi-
ciency of alum at various pH was measured in terms of
turbidity. The studies showed that alum had the best
removal efficiency at pH of 7.5 (Fig. 2). Zeta potential
measurement of effluent treated with alum at various
pH confirmed that the treated colloidal dispersion was
stable at pH 4.0–5.0. However, at pH 7.0–7.5, as the
zeta potential approached zero, colloidal dispersion was
destabilised (Fig. 3).
3.2.1. Optimising chemical dosage
Experiments were carried out to determine the com-
bined optimum dose of alum and polyelectrolyte. First,
the optimum dose of alum was determined. The coag-
ulation and flocculation of wastewater was investigated
using alum doses of 100–1000 mgyl. The pH was kept
constant at 7.5 by using either calcium hydroxide or
sulphuric acid. Coagulated wastewater samples were
tested for residual suspended solids (measured as tur-
bidity) and COD. The results of alum coagulation
treatment for wastewater are shown in Fig. 4. The
studies showed that a relatively low aluminium ion
dosage of 700 mgyl was capable of reducing turbidity
and COD load from the wastewater by coagulation to
an acceptable level. Furthermore, the relationship
between suspended solids and turbidity of the effluent
at various dilutions are shown in Fig. 5. The plot was
generated by diluting the effluent having an initial
turbidity of 1080 NTU with distilled water. Relative
turbidity, TyT0, where T0 is T in the absence of floccu-
lant, was employed as a measure of the efficiency of
the flocculant used. At the optimum dosage of approx-
imately 700 mgyl, the COD reduced by 65% while the
relative turbidity reduced to 12.8% (Fig. 6). Addition
of polymer concentration between 1 and 10 mgyl at
optimum alum dosage of 700 mgyl further enhanced
the COD and turbidity removal. A maximum COD
removal of 74% was observed at a polymer concentra-
tion of 6 mgyl while the alum dosage was kept at 700
mgyl (Fig. 7). Consequently the relative turbidity (Ty
T0) decreased from 12.8 to 0.37%.
4. Cross-flow microfiltration
Cross-flow microfiltration was employed as the pol-
ishing treatment for the effluent to generate microorgan-
460 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466

Table 3
Physico-chemical characteristics of the effluent stream

Parameters Unit Minimum Maximum Averagea Std. Bb

pH 7.3 7.5 7.3 5.5–9.0
BOD5 @ 20 8C mgyl 150 298 291 50
COD mgyl 926 1468 1362 100
TSS mgyl 1068 1128 1080 100
Temperature 8C 29.5 30.2 30.2 –
Turbidity NTU 1180 3740 2325 –
DO mgyl 2.23 2.26 2.25 –
Mercury as Hg mgyl 0.01 0.03 0.02 0.05
Cadmium as Cd mgyl ND (-0.003) ND (-0.003) ND (-0.003) 0.02
Hexa-chromium as Cr6y mgyl ND (-0.02) ND (-0.02) ND (-0.02) 0.05
Cyanide as CN mgyl ND (-0.02) ND (-0.02) ND (-0.02) 0.10
Lead as Pb mgyl ND (-0.02) ND (-0.02) ND (-0.02) 0.5
Tri-chromium as Cr3q mgyl 0.015 0.25 0.02 1.0
Copper as Cu mgyl ND (-0.003) ND (-0.003) ND (-0.003) 1.0
Manganese as Mn mgyl 0.025 0.035 0.032 1.0
Nickel as Ni mgyl 0.01 0.03 0.01 1.0
Tin as Sn mgyl ND (-0.01) ND (-0.01) ND (-0.01) 1.0
Zinc as Zn mgyl 0.033 0.085 0.067 1.0
Boron as B mgyl 0.18 0.24 0.20 4.0
Iron as Fe mgyl 0.20 0.98 0.32 5.0
Phenol mgyl 0.006 0.016 0.008 1.0
Free chlorine as Cl2 mgyl ND (-0.02) ND (-0.02) ND (-0.02) 2.0
Sulphide as S2y mgyl ND (-0.1) ND (-0.1) ND (-0.1) 0.5
Oil and grease mgyl ND (-2) ND (-2) ND (-2) 10.0
a
Average of 20 samples.
b
DOE Std. B parameter limits for discharge of effluent to inland waters below water intake points.

Fig. 2. pH vs. turbidity.

 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466 461

Fig. 3. pH vs. zeta potential.

ism free water for reuse in the manufacturing process.
Preliminary studies were carried out to determine if
cross-flow microfiltration treatment of the effluent with-
out chemical pre-treatment could be employed. Subse-
quently, effluent that had undergone coagulation–
flocculation pre-treatment was passed through the
cross-flow microfiltration unit. The cross-flow microfil-
tration unit consisted of a cellulose acetate membrane
with pore size 0.2 mm. Membrane treatment by cross-
flow microfiltration of the chemically treated effluent
from the WWTP produced permeate that could be
recycled for various uses within the manufacturing plant.
The filtered water, which was free of suspended matter,
bacteria and colloidal matter, was accepted for reuse
thus, reducing water consumption and effluent discharge
to external watercourses.

Fig. 4. Alum dose vs. COD removal.

462 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466

Fig. 5. TSS of the composite effluent vs. NTU at various dilutions.

4.1. Membrane filtration without pre-treatment
Several experiments were conducted without pre-
treatment of effluent water to examine the effectiveness
of membrane filtration to remove COD, turbidity and
microorganisms. Furthermore, the decline of permeate
flux due to membrane polarisation and fouling was also
recorded. Table 4 shows the solids removal efficiency
in terms of turbidity at different feed flow rates. The
solids removal efficiency was 99% or more in all cases.
However, ultrafine pigments and various macromole-
cules present in the paint caused mild turbidity in the
permeate.
Fig. 8 indicates the permeate flux vs. time for 1 h of
operation. There was marginal drop (;5%) in permeate
flux in the first 20 min, followed by a sharp drop in the
next 10 min. This phenomenon was investigated by
suspending the runs at regular intervals and observing
the fouling of the membrane surface visually. It was
observed that it took at least 20 min to develop any
significant fouling layer. Perhaps residual surface charge
on the membrane surface prevented adsorption of foul-
ing materials to any significant level in the first phase
of filtration. Table 4 shows that initial turbidity was
removed effectively from the untreated effluent water
but the permeate flux decreased significantly in the
beginning, followed by a slower long-term decrease.
This phenomenon is shown in Fig. 9 for a feed flow
rate of 200 lyh. This may be due to blockage of the
membrane by colloidal substances present in the was-
tewater. A set of experiments was also performed with
treated effluent (alum and polymer) at different feed

Fig. 6. Alum dose vs. relative turbidity (TyT0).

 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466 463

Fig. 7. Polyelectrolyte vs. COD removal.

Table 4 4.2. Membrane filtration with pre-treatment

Turbidity of influent and permeate (without pre-treatment)

Influent (NTU) Feed flowrate Permeate Removal 4.2.1. Effect of flocculation

(lyh) (NTU) efficiency A set of experiments was conducted with effluent
water at different feed flow rates to study the effect of
45 9.97 99.07
flocculation on the limiting flux of the membrane
1080 54 10.97 99.98
75 10.80 99.00 filtration. It was observed that the limiting flux rate of
filtration increased 100% due to coagulation–floccula-
tion treatment of the effluent water. However, a flux
flow rates to study the removal efficiency of COD on rate decline was observed for chemically treated was-
the permeate flux of the cross-flow microfiltration unit. tewater, but it was not so predominant in comparison to
The limiting flux almost doubled as shown in Table 6 the untreated wastewater.
for feed flow rates varying between 200 and 400 lyh. The permeability of the membrane plays an important
However, the feed flow rate had no significant effect role in the viability of the process. High permeabilities
on the permeate COD, as shown in Table 5. lead to the potential for higher product fluxes. Fouling

Fig. 8. Permeate flux vs. time for untreated effluent. Feed flow rate 200 lyh.
464 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466
Fig. 9. Permeate flux vs. time for treated effluent. Feed flow rate 200 lyh.
of the membrane surface during processing is especially
a problem with liquid processing. It is observed from
Table 6 that the limiting flux for the effluent with
chemical treatment is higher than the one without
treatment by a factor of two or more in all cases. This
may be due to reduction in membrane fouling, which
improved the permeate flux. However, the limiting flux
increased with increasing feed flow rate in all cases
although the improvement was more perceivable for
treated effluent. Permeate flux in cross-flow microfiltra-
tion depends on cross-flow velocity, temperature, feed
characteristics and the geometry of the membrane mod-
ule (Samuelsson et al., 1997). In the present case, the
limiting flux enhancement was caused by higher cross-
flow velocity when the feed flow rate was increased.
This is consistent with the findings of Samuelsson et al.
(1997) for colloidal fouling.
4.3. Scale up of chemical treatment
Using optimum dosage of alum and polyelectrolyte
obtained from the jar test experiments, 10 l of waste-
water was treated. The trial reconfirmed the coagulant
dose obtained in the jar test for optimum removal of
COD and turbidity. Characteristics of the effluent after
Table 5
COD concentration of influent and permeate (without pre-
treatment)
Influent COD Feed flowrate Permeate Removal
(mgyl) (lyh) COD (mgyl) efficiency
45 209 84.65
1362 54 200 85.32
75 205 84.95
coagulation–flocculation treatment employing a com-
bined dose of alum, calcium hydroxide or sulphuric acid
and polymer are shown in Table 7.
4.4. Scale up of cross-flow microfiltration studies
The chemically treated effluent was then passed
through a cross-flow microfiltration unit. The character-
istics of the effluent after coagulation–flocculation and
membrane treatment are shown in Table 8.
5. Microbiological studies
Two effluent samples were tested for microbiological
contamination by a standard method (Miles and Misra,
1938). The samples had been subjected to chemical pre-
treatment and microfiltration as described earlier. At
each stage of treatment, samples were collected and
tested for microbiological contamination. The six treated
samples and a sample of distilled water used in this
work (control) were screened for aerobic and anaerobic
microbial contamination. Screening for aerobic microbes
were conducted by streaking the samples onto nutrient
agar incubated at 25 and 30 8C to detect bacterial
growth and onto malt extract agar incubated at 25 8C
Table 6
Effect of flocculationypre-filtration on limiting flux
Feed flowrate Limiting flux (lym2 yh)
(lyh)
Without treatment With treatment
200 17.45 36.45
300 22.68 43.93
400 27.85 59.18
 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466 465

Table 7
Physico-chemical characteristics of effluent after coagulation–flocculation treatment

Parameters Unit Std. Ba

pH 7.5 5.5–9.0
BOD5 @20 8C mgyl 96.7 50
COD mgyl 354.12 100
TSS mgyl 8 100
Temperature 8C 27.0 –
Turbidity NTU 8.6 –
DO mgyl 7.03 –
Colour True colour units 5 –
Mercury as Hg mgyl 0.012 0.05
Hexa-chromium as Cr6q mgyl ND(-0.02) 0.05
Cyanide as CN mgyl ND(-0.02) 0.10
Lead as Pb mgyl ND(-0.02) 0.5
Copper as Cu mgyl 0.019 1.0
Zinc as Zn mgyl 0.121 1.0
Iron as Fe mgyl 0.10 5.0
a
DOE Std. B parameter limits for discharge of effluent to inland waters below water intake points.

to detect fungi growth. After incubation for at least 48
h the resultant microbiological growth was visually
assessed using the rating scale detailed in Table 9. SIMy
ISA tubes were used for screening of anaerobic microbes
or more specifically SRB. The tubes were incubated at
30 8C and any resultant growth was assessed visually
according to the extent of black coloration. The results
of the screening test are as shown in Table 9. Microbi-
ological growth was observed for samples A1, A2, B1
and B2. Samples A3, B3 and the control showed no
microbiological growth. Positive microbial growth on
malt extract agar plates was identified as bacterial and
not fungi growth. All ISA tubes showed negative results
indicating no growth of SRB. It can be concluded from
the tests above that the chemical treatment alone could
not remove bacteria from the effluent. However, cross-
flow membrane filtration is capable of removing bacteria
to produce water that is of sufficient quality for use
within the plant. The cross-flow microfiltration unit
employing a cellulose acetate membrane with a pore
size of 0.2 mm is capable of removing the smallest
bacteria, Pseudomonas diminuta which has a diameter
of 0.2 mm.
6. Conclusions
The present study shows that chemical coagulation
followed by microfiltration can be implemented for
water recycling in the plant under study. However, based

Table 8
Physico-chemical characteristics of effluent after coagulation–flocculation and membrane treatment

Parameters Unit Std. Ba

PH 7.5 5.5–9.0
BOD5 @ 20 8C mgyl 28 50
COD mgyl 65 100
TSS mgyl 5 100
Temperature 8C 27.0 –
Turbidity NTU 0.3 –
DO mgyl 7.25 –
Colour True colour units 5 –
Mercury as Hg mgyl 0.01 0.05
Hexa-chromium as Cr6q mgyl ND(-0.02) 0.05
Cyanide as CN mgyl ND(-0.02) 0.10
Lead as Pb mgyl ND(-0.02) 0.5
Copper as Cu mgyl 0.006 1.0
Zinc as Zn mgyl 0.10 1.0
Iron as Fe mgyl 0.03 5.0
a
DOE Std. B parameter limits for discharge of effluent to inland waters below water intake points.
466 B.K. Dey et al. / Advances in Environmental Research 8 (2004) 455–466
Table 9
Screening for aerobic and anaerobic microbes
Samples Microbiological growth ratinga:
Nutrient agarb
25 8C 30 8C
A1 6 6
A2 3 4
A3 0 0
B1 6 6
B2 6 6
B3 0 0
Distilled water (control) 0 0
NB
a
Growth rating scale, 0, no growth; 6, dense growth.
b
Nutrient agar for detection of bacteria.
c
Malt extract agar for detection of fungi (including yeast).
d
ISA tubes for detection of SRB.
e
Presence of bacteria.
on the experimental findings, the following conclusions
can be drawn.
1. The efficiency of treatment of paint is strongly
influenced by the effluent pH. In the pH range of
4.0–4.5 the floc formation was minimal, however
when the pH was increased to between pH 7.0 and
7.5 flocs were easily formed. The studies showed
that the optimum pH for the treatment was 7.5.
2. Zeta potential studies confirmed that at pH 7.0–7.5,
the colloidal dispersion was completely destabilised.
As the pH of the treated effluent increased the zeta
potential of the treated effluent approached zero.
3. Effective treatment of the effluent can only be
achieved by employing alum in combination with
polyelectrolytes. Treatability of the effluent improved
with the use of polyelectrolytes in combination with
alum compared with the use of only alum. Maximum
COD and turbidity removal rates of 74 and 99.6%
were recorded.
4. At the pH of 7.5, the optimum dosage of alum was
700 mgyl. The optimum dosage of polyelectrolyte in
combination with alum (700 mgyl) was found to be
6 mgyl.
The present study showed that effluent from the
WWTP could be reused in various operations within
the plant without any risk of microbial contamination.
It was also found that pre-treatment of the effluent was
necessary as untreated effluent had an adverse effect on
the limiting flux of the membrane filtration process. It
Malt extract agarc ISA tubesd
25 8C 30 8C
0 0
3e 0
0 0
6e 0
6e 0
0 0
0 0
was deduced that limiting flux increased by 100% when
the effluent was chemically treated. Microbiological
tests carried out on effluent before and after chemical
treatment and after membrane filtration confirmed that
there is negligible risk of microbiological contamination
in the permeate flux.
References
Anderson, J.E., Springer, W.S., Strosberg, G.G., 1981. Appli-
cation of reverse osmosis to automotive electrocoat paint
wastewater recycling. Desalination 36, 179–188.
American Public Health Association, 1992. Standard Methods
for The Examination of Water and Wastewater, 18th ed.
Briggs, M.A., 1977. Paint Research Association Technical
Report TR14177. Paint Research Association, Teddington,
UK.
Dey, B.K., 1999. Wastewater recycling in a paint manufactur-
ing plant. M.Tech. Thesis, Institute of Post Graduate Studies
and Research, University of Malaya, Kuala Lumpur,
Malaysia.
Miles, A.A., Misra, S.S., 1938. The estimation of the bacterial
power of the blood. J. Hyg. 38, 732–735.
Opperman, R.A., Goll, M., 1984. Presence and effects of
anaerobic bacteria in water-based paint. J. Chem. Technol.
56, 51–55.
Samuelsson, G., Huisman, I.H., Tragardh, G., Paulsson, M.,
1997. Predicting limiting flux of skim milk in crossflow
microfiltration. J. Mem. Sci. 129, 277–281.
Uenoyama, K., Kajino, T., Okai, T., Shibata, T., Koike, T.,
1996. Method for recycling a paint recovery effluent. J.
Cleaner Prod. 4, 79.