PII: S0043-1354(97)00416-8

Wat. Res. Vol. 32, No. 7, pp. 21802186, 1998

# 1998 Elsevier Science Ltd. All rights reserved
Printed in Great Britain
0043-1354/98 $19.00 + 0.00

EFFECT OF CALCIUM ION ON THE FOULING OF

NANOFILTER BY HUMIC ACID IN DRINKING
WATER PRODUCTION
M
SEONG-HOON YOON1, CHUNG-HAK LEE1**
, KYU-JIN KIM2 and
ANTHONY G. FANE2

Department of Chemical Technology, Seoul National University, Kwanak-Gu, Seoul, 151-742, Korea
and 2UNESCO Centre for Membrane Science and Technology, The University of
New South Wales, Sydney 2052, Australia

(First received May 1997; accepted in revised form October 1997)

AbstractThe inuence of the charge of humic acid (HA) on the fouling of nanolters was investigated
as a function of pH and concentration of calcium ions. The charge of the humic acid as well as the
zeta-potential of the membrane surface were measured to elucidate the mechanism of humic acid deposition on the membrane surface. The negative charge of humic acid as well as the negative zeta-potential of the membrane surface fouled with humic acid increased with higher pH. As a result the further
deposition of humic acid on the membrane surface was expected to decrease with higher pH because of
larger repulsive forces. With moderate calcium ion concentration, however, the adsorption of humic
acid onto the membrane surface decreased until neutral pH and then increased again. It was attributed
to calcium ion bridging between two free functional groups of humic acids. Calcium ion rejection
decreased in the presence of humic acid deposited on membrane surface. This could be explained by
the eect of humic acid on the net charge of the membrane. The addition of calcium chelating agent,
EDTA, improved ux, especially at alkaline conditions. The diagram of CaEDTA vs pH was used to
explain the ux improvement. # 1998 Elsevier Science Ltd. All rights reserved
Key wordshumic acid, nanoltration, calcium ion, zeta-potential, EDTA

INTRODUCTION

Membrane fouling caused by organic matter has

been generally experienced in surface water ltration plants for the production of drinking water
as well as process water (Thorsen, 1993). Humic
materials, which form a major organic constituent
in surface water, has been considered to be a signicant foulant (Nystrom et al., 1996).
Humic materials are ubiquitous in the aquatic environment and are degradation product of lignin,
carbohydrate and protein, etc. Humic materials are
coiled, long-chain molecules which may be slightly
crosslinked. Their electric charge, derived mainly
from the ionization of carboxyl groups, results in
mutual repulsion and expansion of the coil
(Stevenson, 1982). According to Cameron et al.
(1972), a random coil is the most likely structure of
dissolved humic acid. Ghosh and Schnitzer (1980)
proposed that both humic and fulvic acids are most
densely coiled at high concentration, low pH, or at
raised ionic strength, I, and at low ionic strength,
neutral pH and low concentration, the macromolecules behave like exible linear colloids. As a result
*Author to whom all correspondence should be addressed
[Fax: +82-2-888-1604].

physical and chemical property of humic acid could

vary signicantly at dierent conditions (Cornel et
al., 1986).
It is known that inorganic ions can contribute to
the adsorption of organic materials on surfaces
(Stevenson, 1983). In terms of membrane fouling by
humic materials, Jucker and Clark (1994) investigated the eect of the ionic strength of solution on
humic acid adsorption onto ultraltration membrane surface for various pH and ionic strength. It
was found that the amount of adsorption increased
with lower pH and higher ionic strength. Hong et
al. (1996) found that ux decreased with higher
inorganic ion concentration. Nystrom et al. (1996)
has investigated the eect of copper ion on membrane fouling using soil born humic acid for various
kinds of lters at various ltration conditions. It
was suggested that the fouling should be aected by
the binding tendency of humic acid with copper
ion. As a result of the above, it has been considered
that the charge interaction between membrane surface and humic material with or without inorganic
ions is a major mechanism of membrane fouling
and anti-fouling. However, few studies have been
done on the quantication of humic acid charge or

2180

Fouling of nanolter by humic acid

the eect of the calcium ion on membrane fouling

by humic materials.
In this study, humic acid and calcium ion commonly found in surface water were used to investigate the eect of inorganic ion on nanomembrane
fouling by organic materials in drinking water production. The charge of the humic acid was
measured by potentiometric titration at dierent
pH and calcium ion concentration. The zeta-potential of the membrane surface was also measured
with and without humic acid. The amount of
adsorbed humic acid on the membrane surface was
estimated to investigate the eect of calcium ion
concentration on humic acid adsorption at dierent
pH. The eect of calcium chelating agent on the
ux was also studied.

EXPERIMENTAL

Materials and method

Water born humic acid (Suwannee river, U.S.A.) was
obtained from International Humic Substance Society
(IHSS). The reported chemical parameters of the humic
acid are summarized in Table 1. The powdered humic acid
was dissolved in water without further purication and the
concentration of 18.5 mg/l (10 mg/l as TOC) stock solution was made. The stock solution was stored in a refrigerator at 48C and diluted to 13 mg/l (7 mg/l as TOC)
before use.
All chemicals used were analytical reagent grade produced by Ajax Chemical. Hydrochloric acid and sodium
hydroxide were used to adjust pH of the solution and
sodium chloride for ionic strength. All experiments were
performed at zero ionic strength(no additional salt added
to adjust ionic strength) or 0.01. The water quality was of
conductivity <1 mS/cm.
A stirred cell made of stainless steel was used at 10 bar
in this experiment. The diameter of the stirred cell was
52 mm and the volume was 160 ml. The stirring speed was
xed at 230 rpm. Filtration was performed until 130 ml of
permeate was eluted in each experiment. The concentration of calcium ion was measured in the collected
permeate (130 ml) and the rejection was calculated as
(1 [Ca2+]permeate/[Ca2+]initial). Figure 1 shows the schematic diagram of the experimental device.
The weight of permeate from the stirred cell was
measured on an electronic balance and connected to a
computer for data analysis. Flux decreased from around
70 to around 40 l/m2/h while feed solution was concentrated from 160 to 30 ml. Average ux was used because
most of the ux decline followed a similar pattern and
comparison of ux at any particular moment was considered to be improper. The average ux was calculated by
averaging the ux which was obtained when feed solution
was concentrated from 160 to 30 ml.
Table 1. Reported characteristics of IHSS reference humic aid
Molecular weight
Diusion Coecient
Carboxyl group
Phenolic group
Total acidity
a

1,490 (number average)a

3.23  106 cm2 s1 a
4.0 meq/gb
2.9 meq/gb
6.9 meq/gb

4.9 meq/gc
2.9 meq/gc
7.8 meq/gc

Beckett, 1987, all the values are of peak maximum in ow eldow fractionation method.
Jucker and Clark, 1994, potentiometric titration data.
c
Thorn, 1989, 13 C NMR data.
b

2181

Fig. 1. Schematic diagram of stirred cell device.

A MPF-34 composite nanolter (Weizmann, Israel) was
used because it has a wide pH tolerance. The NaCl rejection of the nanolter is reported to be 35% by manufacturer and the water ux was measured to be 7080 l/m2/h
at 10 bar. Prior to the ltration all new membranes were
thoroughly cleaned to remove remaining organic and inorganic materials by successively ltering 0.1 M sodium hydroxide and 0.1 M hydrochloric acid solution at 10 bar.
Finally the membrane was cleaned with ultrapure water.
The used membrane was cleaned by the same method as
initial cleaning. The room temperature was maintained at
23228C.
Calcium chloride was used as divalent calcium ion
source. The added calcium concentration was up to
80 mg/l (2 mM). The ash content of the IHSS humic acid
was about 3% and it represents mainly its inorganic content (IHSS, 1996). Thus the inorganic content in initially
prepared solution (13 mg humic acid/l) was estimated to
be below 0.4 mg/l and was neglected because it was much
lower than the concentration of calcium.
Analysis
The concentration of humic acid in the permeate and
concentrate were measured on a Cary 1E UV-visible spectrophotometer (Varian Australia P/L) at 254 nm. Since the
UV absorption of humic acid is sensitive to pH, the pH of
the sample was adjusted to 13 before measurement. The
amount of deposited humic acid was calculated from the
dierence between the amount of initially added humic
acid and the sum of the humic acid contained in permeate
and retentate.
The spectrophotometric method of Hach (method 8030)
was adapted to measure the calcium ion concentration in
the permeate. Permeate was diluted accurately and then
indicator and base were added. The base-treated sample
was divided into two and one drop of EGTA (ethyleneglycol bis(b-aminoethylether)-N,N,N',N'-tetraacetic acid) solution was added to one solution. The calcium ion in the
sample can be expected to be completely complexed with
EGTA because the formation constant, Kf, of calcium and
EGTA is known to be very large (=1011, Cristian, 1994).
From the dierence of visible absorption (522 nm)
between the solutions with and without EGTA, calcium
ion concentration was obtained.
The measurement of the streaming zeta-potential of
membrane was carried out in a at-sheet cross ow modules (Nystrom et al., 1994; Kim et al., 1996) made of polycarbonate to suit membrane sample areas of 33.4 cm2,
tted with reversible silver/silver chloride electrodes on
both ends of the membrane. The electrolyte was 102 M
NaCl solution, adjusted in the pH range of 2.57 by addition of small amounts of NaOH or HCl, and maintained

2182

Seong-Hoon Yoon et al.

at 258C in a waterbath. Streaming potential was measured

at ve pressures in the range of 0.5 to 1.5 bar.
The apparent zeta potential, z, was determined from
the slope of DE vs DP plots using the Helmholtz
Smoluchowski equation.
DE=DP e0 er z=Zk

where DE and DP are the developed potential and the

pressure dierence between both ends of the test module.
Additionally, Z is the viscosity of the solvent, k conductivity of the electrolyte in the pores (approximated as bulk
conductivity), e0 the permittivity of vacuum and er the
relative dielectric constant of the electrolyte.
Titrations
Titrations of humic acid solution (100 mg/l, 50 ml) were
performed with 1 N NaOH solution. The ionic strength of
0.01 was adjusted with NaCl stock solution. The total
amount of acidic groups of humic acid, CT, was determined by conductometric titration (Seki and Suzuki,
1995). To remove CO2 from the solution, nitrogen gas was
continuously bubbled through the system. Potentiometric
titration was performed to estimate average dissociation
constant of ligand, a, using autotitrator (736 GP Titrino,
Metrohm, Switzerland). The number of protonated acidic
groups on humic acid was determined from the dierence
between the bulk proton concentrations in the presence
and in the absence of humic acid. Perdue and Lytle (1983)
derived equation 2, assuming ligands in humic acid have
continuous pKa values. In his model, the distribution of
the pKa values can be described by Gaussian distribution.
Consequently the characteristics of the dissociations of
ligands in humic acid can be described by the average
value of pKa(m) and the standard deviation (s).
2 

 
1 
1
10pKa
1 m pKa
dpKa
a p
exp

s
2
s 2p 1 10pKa H
2
Using the m and s, calculated by nonlinear regression
method, average dissociation, a (=dissociated functional
group/total functional group), can be obtained at any pH.
The calcium binding property was investigated by the
potentiometric measurement (Dempsey and O'Melia,
1983). Calcium selective ion electrode (AES602, Activion)
was used.

RESULTS AND DISCUSSION

Fig. 2. Experimental dissociation constant as a function of

pH obtained by potentiometric titration and a simulation
curve which assumes continuous pKa values of the ligands
(Perdue and Lytle, 1983).

charge density of humic acid can be obtained from

the dissociation constants as a function of pH and
the total charge of humic acid.
The amount of calcium ion complexed with
humic acid was determined from the dierence
between the bulk calcium concentrations in the presence and in the absence of humic acid. Figure 3.
shows the amount of calcium associated with humic
acid as a function of total calcium concentration.
Flaig et al. (1975) found that there is no signicant release of proton when humic acid binds calcium ion. As a result, we can obtain the net
negative charge of the humic acid by subtracting
the charge of the calcium ions binding with humic
acid (Fig. 3) from the initial charge of the humic
acid (Fig. 2). The net charge of the humic acid
increases with pH and decreases with calcium content as shown in Fig. 4.
The above results about the characteristics of
humic acid are summarized in Table 2.

Charge of humic acid with pH and Ca2+ concentration

In conductometric titration of humic acid solution, conductivity would be increased by the
injection of base solution (Seki and Suzuki, 1995).
The increasing rate of conductivity would change
abruptly at the end point. The maximum negative
charge of humic acid was determined to be
6.49 meq/g HA.
A potentiometric titration was performed to estimate the dissociation constant, a, with pH. Figure 2
shows the photentiometric titration result, where
dissociation constant is increasing with pH.
Assuming ligands have continuous pKa values
(Perdue and Lytle, 1983), a simulation curve was
obtained to t experimental data using equation 2.
The average and standard deviation of pKa were
obtained to be 4.24 and 3.84, respectively. The

Fig. 3. Calcium complexation with humic acid as a function of pH (100 mg/l of humic acid).

Fouling of nanolter by humic acid

Fig. 4. Total charge of the humic acid as a function of pH

at dierent calcium concentrations.

Zeta-potential of nanolter
The zeta-potential of MPF34 membrane was
measured with pH and was shown in Fig. 5. The
zeta-potential of unused membrane was positive for
all pHs in the absence of humic acid. However,
when the zeta-potential was measured in the presence of humic acid, it was found to be mostly
negative except at pH 4.5. This phenomenon can be
attributed to the adsorption of negatively charged
humic acid on the positively charged membrane surface. It was assumed that the zeta-potential of
membrane surface would be more negative in the
actual nanoltration process of humic acid because
of the adsorption and deposition of humic acid on
membrane surface.
Flux and humic acid adsorption
Nanoltration of humic acid solution was performed to investigate the eect of charge of humic
acid and membrane surface on the fouling of nanolter. As shown in Fig. 6, signicant ux decline
was observed in the presence of the calcium ion
during the nanoltration of humic acid compared
with that of ultrapure water. On the other hand,
ux decline was not observed in the absence of the
calcium ion.
Except for the case of zero calcium concentration
the ux showed a distinct trend with pH regardless
of calcium concentrations (Fig. 6). The average ux
increased with pH and reached maximum value and
then decreased again. It is worth noting that this
phenomenon is coincident with the trend of
adsorbed humic acid shown in Fig. 7. The amount
of adsorbed humic acid at each pH was mostly

2183

Fig. 5. The eect of pH on the zeta-potential of the

MPF34 membrane, I = 0.01, [HA] = 18.5 mg/l.

inversely proportional to the ux, i.e. it has a minimum plateau.

In the absence of calcium ion, uxes were not so
much lowered inspite of the some amount of
adsorbed humic acid. It was considered that the
deposited layer might have loose structure because
there does not exist calcium ion which connects
dierent humic acids.
Membrane fouling by colloid particles has been
explained by van der Waals force and electrostatic
interaction between the colloidal particles and the
membrane surface as shown in Fig. 8(a). According
to this theory, the amount of humic acid to be
adsorbed should decrease with increasing pH
because the electrostatic repulsion between the
humic acid and the membrane surface would
increase with the increasing pH.
On the other hand, humic acid adsorption caused
by calcium ion bridging between humic acids in solution and in deposited layer would increase with
the increasing pH as shown in Fig. 8(b) because the

Table 2. Measured characteristics of IHSS reference humic acid

Average pKa (m)
Standard deviation (s)
Maximum charge density
Range of charge density

4.24
3.84
6.49 meq/g
26 meq/g

Fig. 6. Average ux as a function of pH at various

calcium ion concentrations during nanoltration of humic
acid.

2184

Seong-Hoon Yoon et al.

Fig. 7. Amount of humic acid adsorbed on membrane

with pH.

Fig. 9. Comparison of mean ux in dierent ionic strength

of zero and 0.01.

number of negatively charged functional group of

humic acid would increase with pH and oers more
binding sites to the calcium ions.
As a result, the amount of humic acid adsorbed
would decrease to some point of pH because of
increasing electrostatic repulsion [Fig. 8(a)] and
then increase again because of the enhanced calcium
ion bridging between negatively charged functional
groups [Fig. 8(b)]. It suggests there exists an optimum pH at which the membrane fouling by humic
acid would be minimum in the presence of calcium
ions during nanoltration.

Calcium ion rejection

The eects of ionic strength

The trend of uxes with pH was similar with the
moderate ionic strength of 00.01 as shown in
Fig. 9. This result is dierent from that by Hong
(1995) who conrmed the ux decrease with ionic
strength. Malcolm (1986) have suggested that the
humic acids extracted from dierent sources have
clearly dierent chemical properties. It is possible
that the discrepancy might come from the dierent
chemical properties of soil born (Aldrich Co.) and
water born (IHSS) humic acid used in this work.

Figure 10 shows the rejection of calcium ion with

pH for the calcium concentration of 20, 40, 60 and
80 ppm, respectively. The rejection of calcium ion
showed a maximum at mid-pH range for all the
Ca2+ concentrations. Expressed as rejection, the
calcium ion rejection decreases with ionic content as
found for most NF membranes.
The fact that rejection of Ca2+ shows a maximum, i.e. Ca2+ permeation shows a minimum,
around the mid-pH range may be explained by the
eect of humic acid on the membrane charge. In
the absence of humic acid, the rejection of Ca2+ is
higher (permeation is lower) as can be seen from
Fig. 11. This is because the virgin membrane has a
signicant positive charge over the pH range and
this would assist Ca2+ rejection due to charge
repulsion between Ca2+ and membrane surface.
Once humic acid is added, however, the membrane
charge would become less positive or even negative
giving a weaker cation rejection. With a higher
amount of adsorbed humic acid, membrane would
be charged more negatively and, thus, Ca2+ rejection would be less. In this context, the amount of
humic acid adsorbed on the membrane surface

Fig. 8. Mechanism of humic acid adsorption. (a) Van der Waals force and electrostatic repulsion and
(b) bridging of calcium ion between negatively charged functional groups.

Fouling of nanolter by humic acid

2185

Fig. 12. Flux improvement by the addition of EDTA.

Fig. 10. The rejection of calcium ion as a function of pH.
Rejection = 1 [Ca2+]permeate/[Ca2+]initial.

(Fig. 7) is, to a certain degree, coincident with the

extent of Ca2+ rejection (Fig. 10), i.e. a higher
amount of deposited humic acid causes lower Ca2+
rejection.
The eect of chelating agent on ux improvement
The ux enhancement was tested in the presence
of a complexing agent with calcium ion such as
EDTA (ethylenediaminetetraacetic acid). As shown
in Fig. 12, uxes were improved when EDTA
equivalent to the calcium ion was added. Although
the improvement was not large at pH 4, it was signicant at higher pH. When a smaller amount of
EDTA, 0.2 mM was added (less than the initial calcium ion concentration of 0.5 mM), the ux
improvement was not observed. This is because
0.3 mM of the Ca2+ ion would still remain, even if
EDTA sequesters the equivalent amount of calcium
ion from solution.

Fig. 11. Rejection of calcium ion with and without humic

acid.

EDTA is a strong chelating agent and the complex formation constant with calcium ion, Kf, is
5.01  1010 (Cristian, 1994). It can chelate an equivalent amount of calcium ion at alkaline conditions
and reduce the free calcium ion concentration in
solution.
Theoretically EDTA can bind the equivalent
amount of calcium ion above pH 7 if there is no
competing chelating agent as shown in Fig. 13.
However, humic acid is another chelating agent
for the calcium ion, although weaker than EDTA.
The capacity for calcium binding of humic acid
has a maximum of 2 meq/g at pH 10 as shown in
Fig. 3, while that of EDTA is 6.8 meq/g at the
same pH. Consequently most of the calcium ion is
expected to exist as CaEDTA complex rather than
CaHA.
CONCLUSIONS

The following conclusions can be drawn from the

present study:

Fig. 13. Calculated concentration of free calcium ion

and CaEDTA complex as a function of pH in the
solution which does not contain humic acid. Initial
[Ca2+] = 0.5 mM (20 ppm).

2186

Seong-Hoon Yoon et al.

(1) The net charge of humic acid at each pH in

the presence of calcium ion was estimated by conductometric and potentiometric titration methods.
(2) Humic acid gains its negative charge with
increasing pH and loses with increasing calcium ion
concentration.
(3) The streaming potential of the nanolter was
positive in the absence of humic acid but became
negative in the presence of humic acid regardless of
pH.
(4) The repulsion between adsorbed humic and
other humic material was expected to increase with
increasing pH for each calcium concentration.
However the adsorption of humic acid was found
to increase again at high pH at constant calcium
concentration. This was explained by calcium ion
bridging between free humic acid and adsorbed
humic acid on the membrane surface.
(5) With the greater humic acid layer deposited
on membrane surface, the calcium ion rejection of
nanomembrane was decreased. This appears to be
related to the eect of humic acid adsorption on
the net charge of the membrane surface.
(6) Flux was improved by the addition of EDTA
which is strong chelating agent for calcium. The
best ux improvement was observed in alkaline
conditions where the competition for Ca2+ favours
the EDTA rather than the humic acid.
AcknowledgementsThe nancial support for this study
was provided by Korea Science and Engineering
Foundation and Australian Research Council. The
authors would like to thank Arto Philajamaki (Chemical
Technology Department, Lappeenranta University of
Technology, Finland) for the measurement of the streaming zeta-potential of the membrane.
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