UF With Coagulant As Pre Filtration

Techneau, 06.
November 2006
Ultrafiltration with pre-coagulation

in drinking water production
Literature review
Techneau, 06.
November 2006
Ultrafiltration with pre-coagulation

in drinking water production
Literature review
© 2006 TECHNEAU
TECHNEAU is an Integrated Project Funded by the European Commission under the Sixth Framework
Programme, Sustainable Development, Global Change and Ecosystems Thematic Priority Area
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Colophon
Title
Ultrafiltration with pre-coagulation in drinking
water production – Literature review
Author(s)
Philipp Meier, Farhad Salehi, Christian Kazner,
Thomas Wintgens, Thomas Melin
Quality Assurance
By Ingo Machenbach
Deliverable number
D 5.3.4
This report is:

PU = Public
Contents
Contents 1
1 Introduction 4
1.1 Requirements for water treatment 4
1.1.1 Surface water 4
1.1.2 Groundwater 5
1.2 Ultrafiltration in general 6
1.2.1 Process description 6
1.2.2 Operating mode and module design 7
1.2.3 Fouling and chemical cleaning 11
1.3 Use of ultrafiltration in drinking water production 11
1.4 Role of coagulation in combination with ultrafiltration in water treatment 13
2 Pre-treatment options 15
2.1 Coagulation 15
2.1.1 Aluminium-based coagulants coupled with UF 15
2.1.2 Coagulation with PACL coupled with UF 17
2.1.3 Comparison of coagulation with iron chloride and aluminium sulphate coupled with
UF 18
2.1.4 In-line coagulation 20
2.1.5 Comparison of in-line and standard coagulation coupled with UF considering the
effect on the removal of DOMs 21
2.1.6 Coagulation coupled with UF with an aerated submerged membrane 24
2.1.7 Coagulation coupled with filtration with metal membranes 26
2.1.8 Summary 27
2.2 Alternative pre-treatment options 27
2.2.1 Adsorption with IOP or PAC coupled with UF and pre-chlorination 27
2.2.2 Pre-chlorination coupled with UF 29
3 Removal capactiy and impact of water quality parameters 32

3.1 Removal of microorganisms with UF 32
3.1.1 Bacteria and Protozoa removal 32
3.1.2 Virus removal 33
3.2 Removal of natural organic matter 34
3.2.1 Effect of ionic strength and pH on humic substances removal 34
3.2.2 Use of additives for a higher specific flux and better humic acid removal 38
3.2.3 Influence of colloidal iron on zeta potential 40
3.2.4 Influence of pH on coagulation coupled with UF with respect to NOM removal 41
4 Fouling control 44
4.1 NOM fouling 44
4.2 Biofouling of UF membranes 53
4.3 Heterogeneous fouling in dead-end UF 55
Ultrafiltration with pre-coagulation in drinking water production – Literature review

© TECHNEAU -1 - November 2006
5 Cleaning procedure for UF membranes 57
5.1 Hydraulical cleaning of UF membranes 57
5.1.1 Air sparging in UF hollow fibres 57
5.1.2 UF in the feed-and-bleed mode (cross-flow) 58
5.2 Chemical cleaning of UF membranes 59
6 Case studies 64
6.1 Roetgen (Germany 64
6.2 Hermeskeil (Germany) 67
6.3 Keldgate (UK) 68
6.4 Switzerland 68
6.5 Minneapolis (USA) 69
6.6 Choa Chu Kang (Singapore) 71
6.7 Iverness (UK) 72
7 Conclusions 75
8 References 77

1 Introduction
In recent years, surface water purification with ultrafiltration membrane has

become an attractive alternative to conventional clarification. No or less need
of chemical agents, good quality of produced water independent of feed
water quality, good removal efficiency towards microorganisms, less
production of sludge, compact process, and easy automation are some of the
advantages of ultrafiltration compared to conventional treatment. Originally,
ultrafiltration was used to remove turbidity and microorganism from good-
quality surface water. Nowadays the main goal is to improve this technology
and to apply it to worse quality sources for the removal of microorganisms,
natural organic matter (NOM), dissolved organic matter (DOC), disinfection
by-products (DBPs), and other components.
In order to accomplish this purpose, many experiments have been conducted
regarding to pre-treatment, membrane operational mode, membrane
material, fouling mechanisms, membrane and water parameters, and the
influence of components of the raw water. The aim of this report is to review
the current practice in employing the ultrafiltration process with pre-
treatment options, mainly coagulation, and to summarise the existing
knowledge of application, including operational experiences. The report also
focuses on the impact of water quality parameters and on the different
reasons and forms of fouling of UF membranes.
1.1 Requirements for water treatment
1.1.1 Surface water
The quality of surface water is determined by hydrodynamic, biological,

chemical, physical and meteorological processes. Intensive rainfall and flood
in the catchments area can cause quite considerable degradation of the
surface water quality [1]. Surface waters contain inorganic and organic
particulate substances. Inorganic particulate constituents are amongst others
clay, silt and minerals. Organic particulate substances can include
microorganism like viruses, bacteria and protozoan [2].
One of the major problems of using surface water as source for drinking
water is the high content of natural organic matter (NOM). NOM can cause
odour, can influence the taste and can increase corrosion and biofilm growth
in the distribution network. Furthermore NOM could be a source for the
formation of disinfections by-products when water is disinfected. Hence,
NOM removal is one of the most important treatment requirements for the
production of drinking water [10]. Fig. 1 shows constituents of dissolved
organic mattes (DOC) in typical surface water. Within the DOC fraction the
humics play an essential role. Other DOC fractions are the higher molecular
polysaccharides and low molecular weight neutrals.

Building
Blocks Acids
245 ppb 159 ppb
Humics
879 ppb
Low-Molecular-Weight-Neutrals
Polysaccharides 278 ppb
104 ppb
Fig. 1: Typical LC-OCD chromatogram of surface water [50]
The essential requirements to the treatment of the surface water are:
• Removal of particles
• Removal of dissolved matter
• Hardness increase and neutralising
• Disinfection
• Removal of micropollutants
The most common method to remove particulate matter and a portion of the
dissolved NOM from surface waters is by sedimentation and/or filtration
following the conditioning of the water by coagulation [2].
1.1.2 Groundwater
Normally the treatment of protected groundwater is less complex than the

treatment of surface water. The most common requirements for treating
groundwater are [1]:
• Aeration
• Neutralising
• Iron removal
• Manganese removal
• Nitrification
Depending on the raw water quality disinfection and organic matter removal
might also be required [1]. In Germany groundwater can be inducted partly
into the drinking water distribution network without treatment [3]. In
catchment areas with high porous grounds, it could come temporary to
microbiological immersions into the groundwater. Additionally in such cases
disinfection can be also required. In the case of spring waters periodical
immissions of coliform bacteria into the water might occur. Furthermore
intensive rainfall and snowmelt can cause higher turbidity in the water [4].

1.2 Ultrafiltration in general
1.2.1 Process description
Ultrafiltration (UF) is a pressure driven membrane process positioned

between nanofiltration and microfiltration [Fig. 2]. The pore sizes of the
membranes used range from 50 nm to 1 nm. Ultrafiltration is typically used to
remove macromolecules and colloids from a solution [5]. The pore size of
ultrafiltration membranes also allows the removal of pathogenic
microorganisms such as bacteria and viruses, whereas microfiltration
removes only bacteria, but not viruses [6]. Typical membrane filtration
facilities demand an operational transmembrane pressure of about 0.4 to 1 bar
in pressurized systems and 0.2 to 0.4 bar in submerged systems [2].
200
100 Reverse
osmosis
[bar]
Nano-
10 filtration
Pressure Δp
Ultra-
filtration
1
Microfiltration
Filtration
0,1
0,0001 0,001 0,01 0,1 1 10 100
Particle size dP [µm]
Fig. 2: Classification of pressure driven membrane processes [6]
Ultrafiltration membranes are mainly made of polymers like polysulfone,

polyethersulfone or polyvinylidene fluoride. The membranes are prepared by
a phase inversion process with asymmetric structure. Fig. 3 shows the
composition of such an asymmetric ultrafiltration membrane.
Fig. 3: Composition of an asymmetric membrane [6]

1.2.2 Operating mode and module design
One of the major challenges in membrane filtration processes is to realise a

high permeate flux. In the case of ultrafiltration, the particles rejected by the
membrane deposit on the membrane surface and form a cake layer. The
consequence is an additional flow resistance and a decrease permeate flux
through the membrane. This effect can be influenced by the filtration
operation mode. In general one can distinguish between static (dead-end-
filtration) and dynamic (cross-flow-filtration) operation mode as well as
submerged membrane systems. In the dead-end-filtration operation mode,
the feed solution flows orthogonal through the membrane (Fig. 4). The
rejected particles are deposited on the membrane surface and form a cake
layer. The filtration resistance increases and the permeate flux through the
membrane decreases with time [6].
feed - raw water pF > pP permeate flux decline
vP ρm
permeate flux
membrane vP 0
permeate - filtrate time t
Fig. 4: Dead-end process [6]
After certain time intervals, the cake layer has to be removed from the
membrane by module flushing. A decline in permeate flux during the
filtration interval usually is undesirable. Therefore, the reduced permeability
is normally compensated by an increase of the feed pressure (Fig. 5) [6].
constant feed pressure pF constant permeate flux vP
module flushing module flushing

m
ρ
F
feed pressure p
permeate flux vP
filtration flushing filtration flushing

intervall time intervall time
time t time t
Fig. 5: Filtration intervals in dead end processes [6]

A commonly applied method for cake layer removal is permeate back-
washing (Fig. 6). For a short-time interval, a pressure increase on the
permeate side forces a flow reversion through the membrane detaching the
feed sided cake layer. Prevalently, a turbulent two-phase cross flow with air
and water is applied to cause high shear forces at the membrane supporting
the cake layer removal. The removed parts of the cake layer are discharged
out of the module by a short cross flow flush on the feed side. Subsequently,
the membrane, now free of a cake layer, is ready for a new filtration interval.
In the long run the module flushing procedures will leave some foulants on
the membrane surface requiring a chemical cleaning in certain intervals.
Minimising the number of chemical cleanings is a main objective for the
optimisation of dead-end processes as permeate back-washing leads to a loss
of already filtered water and thus decreases the total process yield [6].
In order to apply sufficient permeate back-washing pressure a high stability

of the membrane and the module are required. Typical modules for dead-end
operation with permeate back-washing are hollow fibre and capillary
modules (Fig. 7). These modules have the advantage of a high packing
density, i.e. they allow a large membrane area into a small volume. The limit
for increasing packing density is based on the loading capacity of modules for
solid matter. Since all rejected solids deposit on the membrane during
filtration, the danger of module blocking grows with increasing packing
density. In addition, a reliable discharge of solids becomes more difficult with
increasing packing density. Each application requires an optimisation
between packing density and solid loading capacity of the module [6].
removal of fouling layer discharge of solids
fouling layer
detached
fouling layer
permeate
backflush
feedside
Cross-flow
air-bubble
flush
flush
membrane membrane
Fig. 6: Module flushing concepts [6]

capillary membranes pressure tube
feed concentrate
permeate
backflush
fibre diameter
potting 0,5 - 1,5 mm
membrane
Fig. 7: Capillary module for dead-end operation [6]
In general dead-end filtration is limited by the solid matter content in the raw
water. With increasing solid matter content filtration intervals decline and the
risk of module blocking rises. Thus, the module has to be flushed more often.
Since each module flushing consumes permeate and energy, the yield of the
process decreases considerably and energy costs increase. At higher solid
content levels, dead-end processes tend to be ineffective and cross-flow
filtration becomes more interesting [6].
In contrast to dead-end operations, dynamic filtration or cross-flow filtration
operates with a feed flow parallel to the membrane surface. Particles usually
deposit on the membrane forming a cake layer. This cake layer formation is
controlled by the cross flow (Fig. 8). The cross flow generates shear- and
buoyancy forces at the membrane surface. Depending on the feed
components deposited particles can be moved from the cake layer to the bulk
flow. If a partial removal of the cake layer occurs due to a higher cross-flow
velocity this is referred to as a reversible cake layer formation. After start-up
such systems reach a steady state condition where particle settlement and
removal are in equilibrium. A constant cake layer thickness builds up, which
results in a stable permeate flux [6].
Fouling
Feed - raw water p > p
F P
a Reversible
b Irreversible
m
Permeate flux vP ρ
Membrane
vP 0 b
Permeate - filtrate
Time t
Fig. 8: Cross-flow operation [6]

There are cases with steadily but slowly declining permeate flux. One reason
for irreversible cake layer formation is a change in structure of the cake layer,
e.g. when smaller particles deposit in cavities created by larger particles. Such
phenomena make process modelling difficult or even impossible. Like for
dead-end operation a periodical cake layer removal, for example by back
washing, is necessary to maintain stable process conditions [6].
In submerged systems, membranes are dipped into tanks holding the

medium to be filtered. Module housings, such as pressure vessels, are not
required. The driving force in this process is applied by vacuum on the
permeate side. In principle, most module systems can be used for submerged
operations. To date, submerged membranes are available in capillary module
design (Fig. 9). Cake layer control in submerged membrane systems is
accomplished by sparging air into the membrane configuration directly
underneath the module. Rising air bubbles create a shear force on the
membrane as well as a slight movement of the capillary tubes, which adds to
the efforts to reduce the blocking tendency of the system. Nevertheless, these
measures alone are not sufficient to limit the cake layer growth. Thus,
membranes in capillary systems are backwashed in short intervals, whereas
for flat sheet modules the permeate side vacuum is merely switched off.
Operation of submerged systems is therefore similar to dead-end operation.
With a constant driving force, the permeate flux can be illustrated as a saw
tooth curve. Nevertheless, the driving force of the process, i.e. the pressure,
usually is adjusted to keep the permeate flux constant. In contrast to dead-
end operation, submerged membranes can also be applied to treat waters
with high solid loading. One example is the use of submerged systems in
activated sludge reactors of wastewater treatment plants as membrane
bioreactors [6].
Submerged capillary module
filtrate
air bubbles
permeate
capillary
channel
membrane
air inlet
Fig. 9: Submerged membrane system [6]

1.2.3 Fouling and chemical cleaning
The occurrence of natural organic matter (NOM) in surface waters cause very
often fouling on the membrane. NOM includes molecular fragments of
plants, algae, microorganism and particularly humic acids [6].
Physicochemical interactions between retained substances with the
membrane are characteristic for all kinds of fouling. Fig. 10 shows potential
fouling mechanisms. Several substances adsorb on the membrane. Under
normal process conditions this kind of fouling can not be inhibited. The
efficiency of the process will be reduced and the permeability decreases [6].
Irreversible cake layer

Adsorption, compaction
precipitation, inclusion of colloids, etc.
Pore blocking
Particle diameter ~ Pore diameter
Inner pore adsorption

Permeable substances
with affinity to membrane material
Biofouling
Microorganisms in film consisting of EPS
Fig. 10: Potential fouling mechanism [6]
In membrane processes chemical cleaning is very often used to clean the

membranes from the fouling compounds. In Ultrafiltration chemical cleaning
is basically used for two reasons [7]:
• Support of the regular backwash (CEB – chemical enhanced

backwash)
• Intensive cleaning of the membrane to regain the original permeability
( CIP – cleaning in place and COP – cleaning out of place)
In the German drinking water production primarily bases, acids and H2O2 are
used for a CEB, because these chemicals form neither by-products nor raise
the germination. Chemicals like chlorine, citric acid or commercial cleaners
are used in the CIP/COP [7].
1.3 Use of ultrafiltration in drinking water production
In recent years the use of ultrafiltration has rapidly increased in the field of
drinking water production. Stricter drinking water regulations and
requirements for the treatment are creating a rapid growth in use of
membranes to treat more challenging water sources [8]. The filtration with
porous membranes is a young, but worldwide quickly expanding technology

in the drinking water production. Fig. 11 illustrates the almost exponential
growth of application of porous membranes in drinking water production [9].
250.000 500
Number of plants > 8 m³/h

200.000 400
Production capacity [m³/h]
150.000 300
100.000 200
50.000 100
0 0
88
90
91
92
94
95
96
97
99
00
01
02
03
89
93
98
19
19
19
19
19
19
19
19
19
19
19
19
20
20
20
20
Worldwide MF/UF production capacity (kumulativ)
Number of plants > 8 m³/h
Fig. 11: Development of MF/UF plants worldwide since 1988; not comprehensive [9]
Fig. 12 shows the basic process chart of a conventional water treatment plant.
After pre-treatment by coagulation, precipitation, and sedimentation, the
water passes typically two filter stages. These filters are designed to sustain a
satisfactory hygienic drinking water quality under normal conditions. At
times with heavy rainfall often feed water conditions change rapidly and
dramatically and germ removal cannot be guaranteed with a sufficient
accuracy [6]. After the outbreak of cryptosporidiosis in Milwaukee, USA, in
1993 causing more than 400,000 illnesses and 50 deaths, it was determined
that Cryptosporidium oocysts had passed through the conventional water
treatment including rapid granular filters. Through this incident the interest
in membrane filtration with its ability to provide a superior level of filtration
increased rapidly and led to an unbroken boom of membrane application in
water treatment [2].
Pre-treatment / Stabilisation Filtration / Hygienisation
Surface Drinking water

water
2 1
Surface water Drinking water
Filter backwash water
3
Filter backwash water
Fig. 12: Application concepts of membrane filtration for/at drinking water processing [6]

The main advantage of ultrafiltration is its function as a safe barrier for
pathogens even at highly contaminated feed water conditions. In principle
the integration of ultrafiltration into water treatment systems can occur at
different places of the process. The most obvious possibility is to install
ultrafiltration at the end of the conventional process as an extension of
existing water facilities. Due to a very good feed water quality, operational
costs for ultrafiltration are low at this place. Another possibility to apply
ultrafiltration into the conventional water treatment process is after the pre-
treatment step (coagulation step) [6]. An economically interesting possibility
is the application of membrane filtration to treat filter backwash water
produced by flushing of conventional filters (concept 3 in figure 12) or
membrane filters. Water facilities spend up to 10% of the water fed into the
network for filter backwash. Treating filter back wash water is especially
interesting for facilities, where
• disposal cost can be minimised by recycling the filter backwash water

• raw water resources are limited and the reuse of the processed filter
wash water as raw water results in a more efficient utilisation of the
plant capacity.
The reuse of the processed filter back wash water in the process of drinking
water processing today requires a safe removal of pathogens. Membrane
technology offers a feasible option while conventional processes have not
proofed successful. Due to relatively small capacities, filter backwash water
treatment plants often can be incorporated into existing buildings [6].
1.4 Role of coagulation in combination with ultrafiltration in water treatment
In water treatment coagulation serves primarily to reduce turbidity. Further

tasks are the removal of pollutions, which are added on suspended matter
(organic matter, trace compounds), the removal of microorganism (bacteria,
viruses or protozoans) and the removal of dissolved organic and inorganic
matter. Surface waters always contain turbidity and particulate matters. The
separation of particles normally occurs by sedimentation, filtration or
flotation. Colloidal particulate matters must often aggregate to larger flocs by
a pre-coagulation step to remove them by filtration or sedimentation. Fig. 13
shows a typical flow chart for the treatment of surface water and
groundwater [1].

Surface water Groundwater
Colloidal and
precipitation
suspended matters
Coagulation
Sedimentation Flotation
(membrane) Filtration (membrane) Filtration (membrane) Filtration
Fig. 13: Typical plan of the treatment of surface water and groundwater [1]
The combination of the process shown in figure 13 depends from

concentration and types of colloidal and suspended matters as well as the
amount of precipitate. If the concentration of particulate matters is low,
filtration can be conducted without pre-sedimentation, whereas pre-
sedimentation is often applied if the raw water shows a high concentration of
particles. Common coagulants are salts from trivalent iron and aluminium
ions [1] as well as pre-hydrolysed products, such as polyaluminium chloride
(PACL).
The main objective of coagulation process is to aggregate small water

ingredients to larger ones. Thus the removal of such substances by following
applications is possible and easier respectively [1]:
• Advanced removal of colloidal and suspended matters

• Removal of dissolved organic matter (DOC), especially humic acids.
• Removal of inorganic trace metals and phosphate
In the application of ultrafiltration the coagulation can furthermore reduce

fouling on the membrane and enhance the efficiency of the process (see also
chapter 4).

2 Pre-treatment options
2.1 Coagulation
In drinking water production coagulation as a pre-treatment process for

membrane filtration (UF/MF) can enhance significantly the efficiency of the
filtration process, resulting in a higher flux level and increasing NOM
removal [10]. This section describes different coagulation options for pre-
treatment:
• Type of coagulant (aluminium sulphate, PACL, iron chloride)

• Application modes (in-line coagulation, standard coagulation,
submerged membranes, metal membranes)
2.1.1 Aluminium-based coagulants coupled with UF
The type and dosage of coagulant is important for an efficient pre-treatment

in the hybrid process coagulation coupled with UF. Kabsch-Korbutowicz et
al. [11] compared three different aluminium based coagulants to evaluate the
suitability for this process. As residual aluminium in permeate is suspected to
be a causative agent of the neurological disorders such as Alzheimer’s
disease, it was also examined which coagulant had the lowest residual
aluminium.
In this lab-scale study a polyethersulfone membrane and a regenerated
cellulose membrane with MWCOs of 30 kDa were used. Coagulation was
performed in jar test with 3 minutes rapid mixing, 20 minutes slow mixing
and 1 hour of settling. The coagulants tested were aluminium sulphate
Al2(SO4)3 x nH2O (14.3 ≤ n ≤ 15), polyaluminium chloride PAC10WA (basicity
of 60 ± 5%) and sodium aluminate NaAlO2. Dosage was 3.59 g Al/m³ for all
coagulants. Transmembrane pressure (TMP) was hold constantly at 0.1 MPa.
After addition into the water, the Al coagulant undergoes the following
hydrolysis reactions:
Al3+ ←⎯ ⎯ ⎯ ⎯ ⎯
+
→ Al(OH)²+ ←⎯ ⎯ ⎯ ⎯ ⎯
+
→ Al(OH) +2 ←⎯ ⎯ ⎯ ⎯⎯
+
→
+ H 2O , − H + H 2O , − H + H 2O,− H
Al(OH)3 ←⎯ ⎯ ⎯ ⎯ ⎯ → Al(OH) −
+ H 2O , − H +
4
The pH-level, Al ion concentration, temperature and the presence of other

ions influence the reactions and the properties of the produced species.
Monomeric products like Al3+ and Al(OH)2+ may be detected as well as
polymeric products like Al2(OH)3 and Al(OH)4-. The polymeric products with
high positive charge are more likely to occur if pre-hydrolyzed coagulants
(PAC) are used. It was detected that a larger size of pre-hydrolyzed products
leads to a higher probability of their collision with the organic colloids and a
better retention by the UF membrane [11].

Table 1: Effect of the aluminium coagulant type on the colour and the SUV254 removal efficiency in the
coagulation / UF process for the PES and the C membrane [11]
coagulation coagulation/PES coagulation/

membrane C membrane
RColour [%] RSUV254 [%] RColour [%] R SUV254 [%] RColour [%] RSUV254 [%]
UF - - 52.7 46.8 32.2 27.1
Al2(SO4)3 49.2 50.0 89.0 82.1 85.2 78.9
PAC 10WA 57.1 48.2 92.3 84.2 82.2 75.4
NaAlO2 39.6 28.4 59.8 48.5 55.9 43.7
Fig. 14: The effect of the coagulant and the membrane type on the TOC removal efficiency [11]
Table 1 and Fig. 14 show that the best performance regarding TOC, colour,
and SUV254 removal was achieved with the PES membrane with Al2(SO4)3 and
PAC 10WA as coagulant. When sodium aluminate was used as coagulant, in
all cases the efficiency was lower. In the case of coagulation with sodium
aluminate prior to the filtration with the PES membrane the removal
efficiency was lower than the PES filtration without pre-coagulation. It also
leads to an increase of pH, which resulted in an increase of the dissociation
degree of the NOM particles. Concurrently the quantity of positively charged
products of the coagulant hydrolysis decreased. Hence, the elimination rate of
organic matter particles was reduced.
The dependence of the residual aluminium on the coagulant type was
investigated by measurements of permeate (Fig. 15).
The lowest aluminium residual was measured when the pre-hydrolyzed
coagulant PAC 10WA was used. Similar values were reported if 'alum'
(Al2(SO4)3) was used. A very high residual, thus the worst result, was noticed
when the coagulation was performed with the sodium aluminate. Both
membranes caused a decrease in the residual aluminium for all tested
coagulants.

Fig. 15: The effect of coagulant type on the concentration of the residual aluminium [11]
In general, regarding the removal rates and the residual aluminium, PAC
10WA and Al2(SO4)3 as coagulants showed a good performance. Sodium
aluminate cannot be recommended as suitable agent for coagulation coupled
with UF [11].
2.1.2 Coagulation with PACL coupled with UF
The dosage and the type of coagulant used in a study provide different
results with regard to flux decline. One coagulant, which can be used, is
polyaluminium chloride (PACL). Xia et al. [12] used polyacrylonitrile (PAN)
membranes with a MWCO of 50kDa to investigate the best dosage. The raw
water was filtered inside-out in cross-flow mode. Every 30 to 80 minutes the
membranes were backwashed for 45 seconds. The raw water had a turbidity
of 23.0 NTU (Nephelometric Turbidity Unit).
Fig. 16: Effect of coagulant dose and sand filtration on UF flux [12]
As shown in Fig. 16, dosing 1 mg/L and 2 mg/L of PACL had only little
impact on the flux compared to dosing no coagulant and direct UF. With a

dosage of 3 mg/L and more the permeation increases. This was due to the
formation of flocs with sizes preventing fouling of pores. The optimal dosage
of PACL in consideration with the high costs of the coagulant could be
determined as C = 3 mg/L. Xia et al. [12] also compared the coagulation-UF
process and the coagulation - sand filtration - UF process. In this process, the
large size flocs were retained by sand filtration and the small size colloids are
embedded in the same sized pores. This resulted in membrane fouling. With
no sand filtration used, the flocs formed an easily removable and permeable
layer on the membrane where colloids, algae, and other suspended matter
were trapped and adsorbed. In all tests carried out, an effective turbidity
removal with an average of 0.1 NTU was provided [12].
2.1.3 Comparison of coagulation with iron chloride and aluminium sulphate coupled
with UF
Different coagulants are used for pre-treatment in the process combination

with UF. The most common ones are iron based and aluminium based
coagulants. Müller et al. [13] compared coagulation with iron chloride and
with aluminium sulphate coupled with UF. The membrane used for this pilot
scale study was an submerged membrane with a MWCO of 200 kDa in the
outside-in mode. The effect of intermittent air bubbling on the process was
also investigated.
Three different process parameters were tested regarding permeability
decline (Table 2) [13]
Table 2: Survey of process parameters [13]
Phase Raw water Coagulant Aeration parameter

VP 1 bank filtrate; without aluminium sulphate 1 min aeration / 2 min intermission;
aeration 1,0 mg Al³+/L 0,5 m³/(m²·h)
VP 2 bank filtrate; without aluminium sulphate without aeration during filtration
aeration 1,0 mg Al³+/L
VP 3a bank filtrate; aerated 1,5 mg Fe³+/L without aeration during filtration
VP 3b bank filtrate; aerated 2,0 mg Fe³+/L without aeration during filtration
VP 3c bank filtrate; aerated 4,0 mg Fe³+/L without aeration during filtration
Fig. 17 presents the results of the different tests. VP 1 and VP 2 showed that
intermitted aeration had not a large influence on the permeability. Therefore,
it could be considered as inefficient for ultrafiltration with submerged
membranes. If iron chloride was used as coagulant, the phenomenon of
permeability decline was much lower than for aluminium sulphate as
coagulant. The reason for this was presumably the different formation of
flocs, as iron flocs were larger than aluminium hydroxide flocs and had a
lower density. Therefore, they formed a more complex and permeable cake
layer on the membrane surface. The higher the dose of iron chloride (VP 3a to
VP 3c) the lower the decline of permeability was due to higher removal of
dissolved and colloidal matter. Permeate turbidity was constantly below 0.1
NTU. Bacteria and pathogenic germs were completely retained. Residual
coagulant was below the detection limit [13].

Fig. 17: Decline of permeability at different process parameters [13]
Müller et al. [13] showed that pre-treatment with iron chloride was more
efficient than coagulation with aluminium sulphate.
Schippers et al. [14] preferred iron instead of aluminium as coagulant because
of the difficulties with the aluminium sludge and the high cost of this
coagulant. In contrast with other researchers, they determined the best pH-
value was 8 with an iron dosage of 1 mg/L [14]. Schäfer et al. [15]
investigated the influence of ferric chloride pre-coagulation to the membrane
fouling behaviour. They showed that precipitated colloids can cause
membrane fouling by pore blocking or cake deposition. Fig. 18 illustrates the
flux decline over permeate volume for different ultrafiltration membranes
and different ferric chloride concentrations. The flux decreases with
increasing ferric chloride concentration and with higher molecular weight cut
offs (MWCO). An explanation for this phenomenon could be that more open
membranes with a higher initial flux J0 are more sensitive to cake formation
[15].
Fig. 18: Ferric chloride addition in ultrafiltration (100, 30 and 10 kDa membranes, 0,5 mM CaCl2, pH
7-8, 1 mM NaHCO3, 20 mM NaCl, 5 mg/L DOC IHSS FA). [15]

2.1.4 In-line coagulation
In-line coagulation means the use of coagulants without any sedimentation or

pre-filtration of coagulated solids prior to UF. Guigui et al. [16] investigated
the overall performance of in-line coagulation coupled with the UF process in
terms of permeate quality and membrane fouling.
Jar-tests demonstrated that ferric chloride as coagulant provided the best
NOM removal efficiency. A pH of around 5 to 6 led to the highest DOC
removal while a pH about 6 to 7 induced the highest UVA254 removal. This
was due to the higher positive charge of the hydrolyzed metal species at a pH
about 6, which might have reacted with the negatively charged NOM.
Under any coagulation condition, SUV254 removal was greater than DOC
removal during the in-line coagulation coupled with UF process tests. The
best operational conditions determined in the jar-test led to a good
performance of the laboratory dead-end filtration in terms of water quality.
Cake resistance increased at high coagulant doses. The floc cake on the
membrane could retain the uncoagulated NOM and the smallest flocs, which
otherwise could promote fouling. The specific cake resistance grew with
increasing TMP. The cake compression was reversible because with
decreasing TMP the specific cake resistance decreased as well. The cake
resistance depended on floc size and cake porosity [16].
Choi et al. [17] performed further studies on in-line coagulation. They

employed different dosages of alum as coagulant and polyethersulfone (PES)
flat sheet membranes with a MWCO of 100 kDa.
Fig. 19 shows the zeta potential (ZP) as a function of pH and coagulant dose.
The ZP is used to identify the charge neutralisation and sweep floc zones for
conventional and unconventional under-dosed treatment. Charge
neutralization is known to be effective in conventional treatment when ZP is
close to zero (±5 mV). Sweep floc is identified as the zone where at least 90 %
of turbidity was removed by settling. Sweep floc conditions are at a pH
between 6.5 and 8 and a coagulant dose around 3 mg/L as Al. This zone can
vary with changing concentration, contaminant types, and coagulant types. In
this zone, flocs grow large enough to settle down rapidly. During under-dose
conditions, the particles will not form any floc that is able to settle down nor
will they stick to sand or any other media in a rapid filter. Choi et al.
investigated six different conditions. #1 to #3 represents under-dosing
conditions with slightly alkaline (#1), alkaline (#2) and acidic pH (#3).
Conventional coagulation was represented by charge neutralisation (#4), and
sweep floc conditions (#5 and #6) [17].

Fig. 19: Zeta Potential. Blue zone: charge neutralisation conditions; red zone: sweep floc conditions;
green zone: under dosed conditions [17}
The particles formed under conditions #1 and #2 were so small that more
than 85% of turbidity passed through a 0.2 µm membrane filter. All other
conditions showed good removal efficiencies.
Transmembrane pressure (TMP) measurements during in-line coagulation
revealed a rapid increase for the unconventional conditions (#1 and #2) as
permeate flux increased. This was due to pore blocking or development of a
dense and impermeable cake on the surface of the membrane because under
these conditions the particles had the smallest size. The best TMP
performance was observed at condition #3 (under-dosing with acidic pH) and
#4 (charge neutralisation). The relationship between TMP and flux was linear
for these conditions.
Backwash efficiency was better for charged particles than for the destabilized
particles that were formed during conventional treatment. A larger absolute
value of ZP resulted in more effective hydraulic cleaning.
Summarizing the tests the under-dose condition #3 with acidic pH showed
the best performance since it was possible to obtain good removal rates of
contaminants and improved physical performance. Moreover, less waste
solids were produced when the low amount of coagulant was dosed. As
proved by the application on different waters the absolute values of
coagulant dose and pH depend on the nature of the raw water and on the
operational requirements [17].
2.1.5 Comparison of in-line and standard coagulation coupled with UF considering the
effect on the removal of DOMs
Dissolved organic matter (DOM) in raw water can cause serious fouling on
the surface of the membrane. Coagulation as a pre-treatment before UF is
known to remove DOMs and therefore reduce fouling. Park et al. [18]
examined the two different ways of coagulation, namely in-line and standard
coagulation, with respect to the removal of DOM and membrane

performance. Cross-flow as well as dead-end filtration was conducted.
Moreover, they examined the effect of pre-coating of the membranes with
metal hydroxide particles of coagulants to advance the coagulation + UF
system.
They used a polyethersulfone (PES) hollow fibre membrane with a nominal
pore size of 0.01 µm in the inside-out mode. Polyaluminium chloride (PACL)
was used as the coagulant at a concentration of 1.0 - 10 ppm as Al2O3. Batch
experiments determined the most effective dosage was 4.1 ppm as Al2O3. As a
comparison, ferric chloride was also used. Flux was hold constantly at 100
L/m²h. In contrast to the dead-end mode, the water was circulated in the
cross-flow mode. Backwashing was executed for 1 min at 1h intervals in the
cross-flow mode and for 20 s at 20 min intervals in the dead-end mode.
Pre-coating was done as follows: Aluminium hydroxide particles were
prepared for pre-coating by diluting a PACL stock solution with ultra pure
water and adjusting the pH to 7.0 (± 0.2). The slurry was dosed to the feeding
line to form a permeable and easily removable coating layer on the membrane
surface, which was predicted to remove DOMs by adsorption. Since this layer
was removed with every backwash, the slurry was dosed for the first 1 min of
every 20 min cycle.
As shown in Fig. 20 membrane filterability was better for standard than for
in-line coagulation and best at a PACL dosage of 10 ppm. Membrane fouling,
caused by particulate matter like coagulated flocs or colloidal matter, was the
reason for the decrease in filterability. Measurements of the particle size
distribution revealed that during the circulation loop of the cross-flow mode
the size of particulate matters became equalized in spite of different
conditions used for coagulation. Park et al. gathered from this that the
removal of DOM was most responsible for the differences in filterability since
particles with a size of over 2µm could not theoretically approach the
membrane surface because of the back transport velocity [18].
Fig. 20: Variation in TMP as a function of coagulation conditions in the cross flow mode [18]
In the dead-end mode (Fig. 21), like in the cross flow mode, ordinary
coagulation and in-line coagulation improved the membrane filterability. Best
improvement was reached with ordinary coagulation. In the dead-end mode,
the flocs remained intact and formed a cake layer. The cake characteristics
varied with the different coagulation conditions. At ordinary coagulation

conditions, the cake was build out of dense and spherical flocs that formed a
permeable cake layer. At in-line coagulation conditions, the cake was build of
loose and elongated flocs that formed a less permeable cake layer. The
difference in filterability appeared to be due to better removal of DOMs and
better floc characteristics during ordinary coagulation conditions [18].
Fig. 21: Variation in TMP as a function of coagulation conditions in the dead-end mode [18]
In the pre-coating experiments with PACL at 4.1 ppm, the filterability was
worse than for ordinary or in-line coagulation conditions. This was caused by
the high resistance of aluminium hydroxide particles. By reducing the dosage,
a better filterability could be reached. Therefore, pre-coating could reduce the
need of coagulant, but the removal of DOMs was not that efficient as in the
other conditions. When ferric chloride was used for pre-coating filterability
increased because the iron hydroxide particles formed a very permeable cake
layer (Fig. 22) [18].
Fig. 22: Comparison of TMP between pre-coating conditions with PACL and ferric chloride [18]
In general, the standard coagulation was superior to the in-line coagulation

and they were both better than pre-coating. Pre-coating should be done with
iron hydroxide particles [18].

2.1.6 Coagulation coupled with UF with an aerated submerged membrane
In a submerged membrane system, the separation step and the coagulation

are conducted in the same tank. To control fouling and therefore stabilize
permeate flux of the membranes, the shear stress has to be raised by using air
bubbling injections. Choksuchart et al. [19] investigated in their lab-scale
study the enhancement of water clarification with an submerged membrane
system and how air injection rates and coagulation conditions can influence
the control of fouling.
Ferric chloride was used as coagulant without pH adjusting of the
suspension. Ultrafiltration was conducted in the outside-in mode. Air was
supplied inside the fibre network at the bottom of each module with an
adjustable airflow rate. The optimal coagulation dose was determined to be in
the range of 0.0 - 0.1 g FeCl3 / g MES. The floc settling velocity was enhanced
by coagulation due to the aggregation of destabilized clay particles [19].
Fig. 23: Microscope analysis of 0.1 – 0.5 g/L clay particles without (left) and with coagulation of 0.01
g/L FeCl3 (right) [19]
Fig. 23 shows that the clay particle size ranged from 55 µm to 70 µm with
coagulation while the size ranged from 11 µm to 20 µm without coagulation.
The critical flux 1 was measured with regard to clay concentration and air
bubbling. Without air bubbling, the critical flux decreased with increasing
clay concentration because of a thick deposit set-up on the membrane surface.
With more air injected a lower critical flux could be obtained (Fig. 24a) [19].
Fig. 24b shows the influence of ferric chloride inside the tank. The clay
suspension was destabilized immediately and the critical flux could be
maintained without air bubbling. At very high concentrations (5 g/L), clay
deposit on the membrane surface was drastic and rapid; hence, air bubbling
was necessary to maintain a stable critical flux. At low concentrations, the
flux remained stable even without air bubbling [19].
1 “critical is a flux value below which there is no or negligible particle deposition on the membrane
surface and above which the deposition is significant during the filtration of suspensions” [51]

Fig. 24: Influence of clay concentration and airflow rate on critical flux a) without coagulation and b)
with ferric chloride dosing [19]
Fig. 25 shows that the large flocs from coagulation (50 µm to 250 µm) were
dissagregated in smaller flocs through air bubbling. Without air induction,
coagulation enhanced the filtration rate due to the larger porosity of deposit.
The flocs were very distant from each other and therefore increased small
particle retention by cake filtration and sorption phenomena. After air
bubbling, the smaller floc size had no consequence on filtration rate [19].
Fig. 25: Particle size (2.0 g/L, 0.2 g/L FeCl3) a) before and b) after 2 h of 50 L/h aeration [19]
With a turbidity removal rate of 95 – 98% a submerged membrane with

coagulation and aeration was proved to be useful in drinking water

production. To optimize the conditions, further studies on the air bubbles
circulation throughout the fibre network have to be conducted [19].
2.1.7 Coagulation coupled with filtration with metal membranes
Polymeric or ceramic membranes are used in most of the studies. Leiknes et

al. [20] tried to investigate if inorganic, sintered metal membranes for UF can
be an alternative to conventional membrane materials.
The membranes for this study were made by Hitachi Metal Ltd. as flat sheets
and had a nominal pore size of about 0.2 µm (measured by the particle size
exclusion analysis). The testing module was build as a plate and frame
system. The membrane reactor was based on a submerged membrane
configuration. Polyaluminium chloride (PAX-16) with a dose of 5 mg Al/L
was used as coagulant at a pH around 6.3 ± 0.2.
First tests with different fluxes showed an increase in TMP after a few hours.
With membrane cleaning, the initial TMP could be restored, indicating that
the fouling was primarily cake formation without particle penetration and
pore blockage of the membrane itself. Backwashing and vigorous air scouring
were applied to reduce the fouling rate, which was due to cake formation.
Different semi sequencing cycles were examined as shown in Fig. 26. The
sludge was extracted before every cleaning period. Scouring of the cake layer
and re-suspending of the solids in the membrane reactor during the cleaning
cycle enhanced flocculation and particle removal whereas fouling was
reduced [20].
Fig. 26: Typical TMP development for the respective 10 and 30 minutes operating modes [20]

The permeate quality was consistent for both cycles. Removal rates of colour
of > 95%, UV254-absorbance around 85% and TOC between 65 – 75% were
within requirements of current drinking water standards. Leiknes et al.
demonstrated that this membrane has a potential for drinking water
treatment. It might be disadvantageous, that inorganic membranes are
generally more expensive than polymeric membranes [20].
2.1.8 Summary
Pertaining to removal rates and residual aluminium, aluminium sulphate and

polyaluminium chloride are better coagulants than sodium aluminate. Iron
chloride is a more efficient coagulant than aluminium sulphate. A pH around
6 is recommended during coagulation. During in-line coagulation, under-
dose conditions with acidic pH showed the best performance because it was
possible to obtain good removal rates of contaminants and improved physical
performance. Nevertheless, ordinary coagulation is superior to in-line
coagulation. Dynamic membranes are a promising alternative to current
techniques applied in drinking water production, because tests showed that
they performed better than membranes with ordinary or in-line coagulation
as a pre-treatment. Metal membranes have a potential for drinking water
production, if the production costs can be reduced. Absolute values of pH
and coagulant dose depend on the nature of the raw water and on the
operational requirements. A direct comparison of the cited test results is
difficult because the studies employed different membrane materials,
operational modes, and raw waters.
2.2 Alternative pre-treatment options
2.2.1 Adsorption with IOP or PAC coupled with UF and pre-chlorination
Instead of dosing a coagulant before UF, the adsorption with iron oxide
particles (IOP) is a possible pre-treatment. It is known that adding IOP into
UF systems increases the NOM removal efficiency and decreases membrane
fouling. However, the interactions between IOP and the membrane have not
been clearly investigated. Ha et al. [21] investigated the characteristics of
adsorptive NOM removal by IOPs in an IOP/UF system with and without
pre-chlorination. To get a better understanding of the efficiency of this
process, they compared it with the removal efficiency of adsorption by
powdered activated carbon (PAC) coupled with UF, which is known to be
helpful in NOM removal. The amorphous IOP slurry (10g/L as Fe) was
prepared in a laboratory by neutralizing a ferric chloride solution using 5 N
NaOH. It had an average surface area of 240 m²/g. The PAC adsorbents had
an average surface of 1400 m²/g. The MWCO of the flat polyethersulfone
membrane was 100 kDa. When they investigate the dosage of both adsorbents
with an adsorption time of 30 minutes, different trends in NOM removal
were found, which was due to the different structures and sorption
mechanisms. Because of high molecular weights, the diffusion of NOM
molecules inside PAC was very low and it took a few days to reach the
adsorption equilibrium. On the other hand, most of the active sorption sites of

nonporous IOP were found on the outer surface layers. The amorphous
structure was widely open to the bulk solution phase. This resulted in a rapid
NOM removal by sorption through surface coordinative reactions, without a
limit on mass transfer. Actually, the initial external mass transfer coefficient
of IOP was with 1.17 x 10-7 m/s almost one order of magnitude higher than
that of PAC (1.26 x 10-8 m/s). Since residence times in these systems had to be
less than a few hours, IOP was the better adsorbent for drinking water
production (Fig. 27) [21].
Fig. 27: Comparison of SUV254 removal efficiency between IOP and PAC adsorbents: adsorption time 30
min [21]
Furthermore, Ha et al. investigated the effect of pre-chlorination on the

adsorption of NOM with IOP. They observed that the SUV254-removal
efficiency decreased with higher dosages of chlorine. This might be due to the
formation of disinfection by products (DBPs) from the reaction with chlorine
and NOM, which were not adsorbable by IOP. Fig. 28 shows that there was a
decline in permeate flux if pre-chlorination was used, presumably due to the
interaction of chlorine with colloidal particles in raw water. The size
distribution changed to smaller particles (Fig. 29) and this made the cake
layer of particles on the membrane denser and reduced the flux.
Fig. 28: Effect of pre-chlorination on flux in IOP/UF and UF alone treating raw water [21]

Fig. 29: Particle size distribution of raw water before and after chlorination: chlorine dose, 11 mg/L;
chlorination time 30 minutes [21]
2.2.2 Pre-chlorination coupled with UF
Groundwater and some water from the anoxic zones at the bottom of
reservoirs often contain Fe2+, and Mn2+, or their complexes with NOM. In
recent years, many water treatment technologies have been tested to remove
these compounds. Nevertheless, these technologies, like a biological trickling
filter, could not meet the WHO guidelines on the Fe and Mn removal, or they
had other disadvantages. Choo et al. [22] investigated a pre-treatment with
chlorination before UF in terms of the removal of iron and manganese from
feed water.
The UF hollow fibre membranes used were made of cellulose and had a
MWCO of 100 kDa. As shown in Fig. 30, there was a rapid increase in
removal efficiency of iron even with a low chlorine dosage of 0.5 mg/L.
Manganese removal efficiency was not as effective. To achieve an efficiency
higher than 40%, at least 2 mg/L as Cl2 had to be added. Hence, a large
amount of chlorine is required if both iron and manganese are present in the
raw water. Choo et al. detected that when a large amount of manganese was
removed by chlorination, serious membrane fouling will occur. At first, it was
assumed that this was caused by the formation of the cake layers on top of the
membrane surface. However, this could not be proved in a UF batch stirred
cell. Surprisingly, they determined that the backwashing was accountable for
the membrane fouling since the concentration of metal oxide particles on the
membrane surface improved the permeability rather than caused fouling,
because these particles could adsorb NOM, which is known as a foulant. The
oxidation of manganese was slower than iron oxidation [22].
Therefore, some of the manganese particles were still small enough to pass
through the membrane pores after chlorination. Afterwards, the growing of
these particles in the pores was assisted by the addition of chlorine during
backwashing, which was done to prevent microbial growth on the membrane

(Fig. 31 and Fig. 32). This was the reason why fouling occurred in this study.
To prevent fouling, backwashing with an acidic solution instead of chlorine is
recommended. Regarding turbidity removal, all tests were successful.
Compared to cross-flow, the performance of dead-end UF was more stable in
terms of the contaminant removal and membrane permeability. However,
membrane fouling was still a problem. The better performance of the dead-
end UF might be due to the formation of uniform deposit layers under even
distribution of transmembrane pressure inside the hollow fibre. During cross-
flow an irregular layer was formed. Thus, dead-end UF with pre-chlorination
is believed to be more practicable [22].
Fig. 30: Removal efficiency of: (a) iron and (b) manganese over time at different chlorine dosages [22]

Fig. 31: Illustration of possible mechanisms of membrane fouling caused by oxidized particles during
pre-chlorination with and without backwashing [22]
Fig. 32: SEM pictures of the UF hollow fibre membranes tested: a) virgin membrane (lumen side) b)
Virgin membrane (shell side), c) used membrane (lumen side) and d) used membrane (shell side) [22]

3 Removal capactiy and impact of water
quality parameters
3.1 Removal of microorganisms with UF
3.1.1 Bacteria and Protozoa removal
Arnal et al. [23] conducted a lab scale study to investigate which UF

membrane is most suitable for drinking water production with respect to
microorganism removal.
In Table 3 the four different tested membranes are given. Experiments were
performed with different feed water with low, medium, and high
microbiological activity.
Table 3: Characteristics of the UF membranes tested [23]
Membrane MWCO [kDa] Material

M1 10 Polyethersulfone
M3 50 Acrylonitrile copolymers
The tests showed that membranes M3 and M4 were very similar in terms of
permeability in spite of their different MWCOs. This was probably due to the
different membrane materials. Acrylonitrile membranes performed better.
Another advantage of this material is that these membranes are more
resistant to free chlorine, which is important when membranes suffer from
biofouling and need a chemical cleaning.
All tested membranes removed the bacteria completely. Fig. 33 shows the
sample of an Enterococcus faecalis assay of feed and permeate for one of the
tested waters. The results were similar for the other permeates.
Thus, all the membranes are suitable for water disinfection.
UF membranes are also used to remove Giardia and Cryptosporidium from
drinking water. Measurements at Hermeskeil (Germany) proved that they
could also be completely removed. (See Chapter 6) [23].
Fig. 33: Microbiological assay of feed and permeate samples [23]

3.1.2 Virus removal
The retention of viruses with low-pressure membranes is dependent on

membrane characteristics, module design, and operational mode. The
efficiency of virus removal can be expressed by a log reduction value (LRV),
which is defined as LRV = log Cr/Cp, where Cr and Cp represent the virus
concentration in the feed and permeate, respectively. Viruses are very small
(10 nm – 400 nm) and can be expected to be completely retained by a UF
membrane with a MWCO of 10 to 100 kDa. Nevertheless, previous studies
demonstrated that the retention could not be predicted only based on
nominal pore size or by the MWCO. It is already known that a more efficient
retention can be achieved with coagulation pre-treatment. Fiksdal et al. (2006)
[24] compared MF and UF virus retention with this kind of pre-treatment.
A polypropylene (PP) hollow fibre membrane with a MWCO of 30 kDa (UF)

and a polyethersulfone membrane with a nominal pore size of 0.2 µm (MF)
were used in outside-in mode in this study. Bacteriophage MS2 was used as
virus in autoclaved tap water because it is similar in size, shape and nucleic
acid to the enteric virus hepatitis A and poliovirus. The coagulants were a
granulated aluminium sulphate product (ALG) and a polyaluminium
chloride product (PAX-16) [24].
Without coagulation, no virus removal was measured for the MF membrane

and only an average LVR of 0.5 log after 60 min was measured for the UF
membrane. This could be due to unusual large pores. Dosing ALG and PAX-
16 improved the LRV with the UF membrane to ≥ 7.1 and ≥ 7.4, respectively.
Similarly high LRVs were obtained with the MF membranes. As comparison,
only a LRV of 2 to 4 can be achieved with conventional water treatment
technologies such as sedimentation or granular high-rate filtration after
coagulation. The aggregation of viruses among each other was not very
important because the pH was around 7. This kind of aggregation occurs
more easily, when the pH is close to the isoelectric point (3.9).
Fig. 34 shows that except the PAX 3 dosage, the MF membrane retained all
viruses because flocs were stable and remained large enough to be retained.
UF showed low virus concentrations in permeate but only the PAX 5 dose
and the ALG 3 dosage could retain all of them. This might be due to the
destruction of flocs during the applied recirculation loop, which was not used
during MF [24].

Fig. 34: The effect of coagulation and filtration through UF/MF membrane on MS2 concentration in
permeate and concentrate vs. type of coagulant dose after 60 min of filtration [24]
As the experiments were conducted in 1h, membrane fouling and inclusion of

viruses into a cake layer on the membrane surface did not play a role.
The average LRVs for all experimental conditions were 6.7. Both UF and MF
membranes with pre-coagulation were efficient hygienic barriers against MS2
virus. Best performance was observed with ALG as coagulant [24].
3.2 Removal of natural organic matter
3.2.1 Effect of ionic strength and pH on humic substances removal
NOM is one of the major reasons causing fouling on the UF membrane. The
major fraction of NOM is humic substances. These substances are negatively
charged when the environmental pH is in the range of natural waters.
Nevertheless, their structure is dependent on the solution chemical
characteristics such as pH and ionic strength. The solution characteristics also
affect the membrane performance, e.g. it can change the membrane surface
charge. However, the membrane pore size is important for the removal

efficiency as well. Costa et al. [25] combined this in a study on the effect of
membrane pore size on the penetration characteristics of humic acid solutions
with different solution chemistries regarding pH and ionic strength. In order
to simulate water with different chemical characteristics, four model solutions
of purified humic acids were prepared at different pH and ionic strength-
levels. The pH was adjusted at 4.5 and 8.2 while the ionic strength was
adjusted to 1 x 10-3 and 1 x 10-2 M NaCl. The membrane characteristics are
shown in Table 4 [25].
Table 4: Membrane characterisation (Lp = pure water hydraulic permeability) [25]
Membrane Lp [kg/(h m² bar)] MWCO [Da] Pore Diameter [nm]

CA1 3.4 2300 2
CA2 50.5 9000 5.4
CA3 65.2 20000 6.2
CA4 100.0 50000 8.6
CA5 164.9 75000 10.6
Membrane permeability tests showed that the solutions with a high ionic
strength of 1 x 10-2 M NaCl had a slightly lower filterability than the solutions
with low ionic strength of 1 x 10-3 M NaCl. From these results, it can be
concluded that salt concentration in the feed water influenced the membrane
performance. Further tests revealed that the tighter membrane CA1 presented
a linear variation of the flux as a function of the operating pressure. The same
was discovered for CA2 and CA3 membrane. Fig. 35 also demonstrates the
decrease of flux with increasing ionic strength at both pH-levels. This can be
explained by the conditioning of the membrane due to adsorption of Cl- ions
[25].
Fig. 35: Permeate fluxes of humic acid model solutions. Membrane CA1; operating conditions:
circulation rate, 200L/h, temperature 25°C [25]
On the other hand, the membranes with the highest pore size displayed a
non-linear variation of the permeate flux as a function of the TMP (Fig. 36).
After cleaning with deionised water, the membranes did not recover the flux

that they reached before the test. This was due to an irreversible fouling layer
caused by humic acid deposition.
Fig. 36: Permeate fluxes of humic acid model solutions. Membrane CA4 (a) and CA5 (b); operating
conditions: circulation rate, 200L/h, temperature 25°[25]
The balance between the convective transfer of humic macromolecules

towards the membrane and the back diffusion influenced the humic acid
membrane deposition as well as the membrane / humic macromolecules
electrostatic interactions. The dominance of convection over diffusion
increased with increasing TMP. For the more permeable membranes CA4 and
CA5, the convectional fluxes exceeded the diffusional fluxes by several orders
of magnitude and the membrane / humic solutes interactions decreased with
increasing permeability of the membranes. As a result, this led to humic acid
deposition and flux decline. For both values of pH, the flux decline was more
distinctive at the higher ionic strength, but the effect of pH was negligible.
Ghosh and Schnitzer [26] and Cornet et al. [27] explained this as follows: At
low ionic strength, humic substances are flexible linear macromolecules,
while at high ionic strength with decreasing thickness of the electrical double
layer of the humic macromolecules, they present lower charge and are rigid
and compact. Hence, these more compacted humic macromolecules will
cause denser fouling layers and pore blocking.
Furthermore, it is reported that the compression of the electrical double layer
at high ionic strength leads to a charge reduction of humic macromolecules
and membranes. This results in a decreased repulsion between the membrane
and humic macromolecules and favours a deposition of these humic
macromolecules on the membrane surface.
Along with the higher capability of convective transport of aggregates to the
membrane surface, the formation of less charged humic acid aggregates is
important for the fouling on the membranes that are more permeable.
Recapitulating, permeation characteristics of humic acid solutions are
dependent on membrane pore size and ionic strength but not on the
solution pH. Furthermore Saravia et al. [28] investigated the influence of the
membrane charge and the charge of suspended solids on the removal
efficiency. Tests were conducted with a negatively charged hydrophilic

hollow fibre membrane with a nominal pore size of 0.035 µm in cross-flow
mode. They used three model substances: a negatively charged polymer, one
with neutral charge and the last polymer with electro neutral charge. These
substances were diluted in water to achieve a DOC content of 3.3 mg/L. The
best DOC removal results were achieved with the negatively charged
polymer at a low ionic strength. With increasing ionic strength, the removal
efficiency decreased due to screening of membrane surface charge and of
charge of the polymer. In the case of the neutral polymer a higher ionic
strength led to a shrinking and clew-building of the polymer. This, together
with the reduced repulsion of the membrane and the polymer caused low
removal efficiency. An increase in ionic strength caused further decrease. The
third solution with the electro neutral polymer showed no removal of DOC
because the molecules were small enough to pass through the membrane.
An increase in ionic strength neutralized the negative surface charge of the
membrane and reduced the charge repulsion of functional groups in the
pores. Domany et al. [29] investigated the removal efficiency of humic
substances by focusing on the MWCO. Table 5 shows the membranes that
were tested.
Table 5: The characteristics of investigated membranes [29]
Membrane Material MWCO [kDa] Pure water flux [L/m²h]

M1 Polyethersulfone (PES) 100 222.2
M4 Poly-aril-ether-ketone (PAES) 5 76.1
Experiments were carried out with deionised water, a humic acid solution
and well water from Senta, Serbia.
Fig. 37: Humic acid concentration in the permeate measured with UV absorbance, DOC and TOC [29]
Fig. 37 shows that the permeate concentrations were almost one order of
magnitude lower than the feed concentrations for all membranes. The

rejection towards humic and organic substances was high. The concentrations
were almost constant with membranes with a MWCO of around 20 kDa and
lower. All the membranes tested were suitable for the removal of humic
substances with removal rates from 85 to 90 % in case of the model solution.
A pre-treatment or membranes with lower pore size could improve the
results [29].
3.2.2 Use of additives for a higher specific flux and better humic acid removal
Polyethersulfone (PES) membranes have excellent chemical resistance, good

thermal stability and mechanical properties. However, they often cause
serious fouling [30]. Qin et al. [30] tried to use LiNO3 and 1,2-PD as additives
to enhance flux and improve the removal of humic acids. Membranes H1,
H2a (Fig. 38), H3a or H3b with an outer skin were fed from out side to lumen
side. H2b (Fig. 39) had an inner skin and the feed water was pumped from
lumen side to out side. The figures demonstrate the different morphology of
the hollow fibre UF membranes.
Fig. 38a) and b) show the finger-like structure of the cross section of the H2a
hollow fibre membrane starting from the outer edge of the fibre through the
whole cross section. The inner edge had 5 µm micro pores (Fig. 38c). The
outer edge of the fibre had no micro pores. This suggested that it had an outer
skin. The inner surface was uniformly micro porous whereas the outer
surface had no visible pores. In contradiction, among other things the use of
an air gap of 600 mm during fabrication produced a membrane with an inner
skin.
Fig. 39 a) and b) show the finger-like structure of the H2b hollow fibre
membrane starting from the inner edge of the fibre and going through the
whole cross-section. The inner edge had no visible pores whereas the outer
edge was fully micro porous with pores of 0.3 µm up to 0.6 µm. The inner
surface had no pores and the outer surface was uniformly micro porous.
Table 6 shows the effect of additive on the specific water flux and on the
retention of humic acid. Other spinning conditions remained almost the same.
For a better comparison, a PES membrane without an additive was
introduced. The addition of 1,2-PG led to an high increase in specific flux.
However, the retention of humic acid was decreased. When LiNO3 was used
as additive, the specific flux decreased as well as the retention. This is due to
larger pores and a thicker skin than the H2a fibre. Table 7 shows that fibres
spun with an air gap performed better than wet-spun fibres. For the H2b fibre
spun with an air gap, both specific flux and retention increased compared to
the H2a fibre even though skin of H2b was only half as thick as the H2a skin.
This could be due to smaller pore sizes of H2b or to thickness errors. The
main difference between the two fibres is the outer skin of the H2a fibre and
the inner skin of the H2b fibre. A small air gap of 2 mm helped to improve the
fibre performance when LiNO3 was used as additive. This could also be due
to a thinner and denser outer skin in case of the H3b fibre compared to the
H3a fibre. In general, fibres with an additive performed better with respect to
specific flux and retention of humic acid than fibres without any additive.
Fibers spun under an air gap had both higher flux and higher retention than
wet spun fibres [30].

Fig. 38: SEM images of PES hollow fibre membrane H2a with an outer skin [30]
Fig. 39: SEM images of PES hollow fibre membrane H2b with an inner skin [30]

Table 6: Effect of additive on specific pure water flux and retention of humic acid [30]
Membrane Used Air gap Specific pure water flux Retention of humic acid
additive (mm) (x 10-5 L m-2 h-1 Pa-1 ) (%)
PES - 0 20 97.4
H2a 1,2-PG 0 93 95.2
H3a LiNO3 0 65 85.0
Table 7: Effect of air gap on performance of the membranes [30]
Membrane Used Air gap Specific pure water flux Retention of humic acid
additive (mm) (x 10-5 L m-2 h-1 Pa-1 ) (%)
H2a 1,2-PG 0 93 95.2
H2b 1,2-PG 600 111 97.4
H3a LiNO3 0 65 85.0
H3b LiNO3 2 96 95.6
3.2.3 Influence of colloidal iron on zeta potential
Iron is often used for coagulation pre-treatment before UF. However, when
coagulation conditions are not optimal, smaller colloidal and soluble iron
species may be present which can affect and clog the membrane [31].
Colloidal iron can also be found in the feed water itself. Soffer et al. [31] used
streaming potential and SEM-EDX (Scanning Electron Microscopy - Energy
Dispersive X-ray Analysis) in their study to investigate fouling interaction of
the colloidal iron with UF membranes and elucidate fouling mechanisms.
They carried out their measurements in a disc ultrafiltration module. Three
polysulfone membranes with MWCO of 10, 30 and 50 kDa and pure water
permeabilities of 22, 35 and 217 L/m²·bar·h and one type F membrane with a
MWCO of 20 kDa and 79 L/m²·bar·h were used. The pH was adjusted in the
range of 2 – 10 during streaming potential measurements using HCl-KOH.
The electrical potential ∆E was measured by varying the applied pressure ∆P
in the range of 10 – 50 kPa. Zeta potential was calculated using the Helmhotz-
Smoluchowski equation:
ΔE / ΔP = ε 0 ⋅ εrζ / η ⋅ k
where ε0 and εr are the vacuum pressure and dielectric constant of the
medium respectively. µ is viscosity of permeate and k is conductivity of
solution. As Fig. 40a) shows, the magnitude of zeta potential is higher for
regular type membranes with a higher MWCO. This is due to changes in the
dielectric constant of water in small pores changing the value of streaming
potential. The 20 kDa type-F membrane had a higher magnitude in zeta
potential at pH ≥7 and a lower one at pH ≤ 6.

Fig. 40b) shows that the zeta potential of all fouled membranes was more
positive than for clean membranes. It can be concluded that most of the
fouling occurs on the surface of the membrane.
As iron is more soluble at acidic pH, the membranes suffered from higher
levels of internal iron deposition at the lower pH.
The higher the negative zeta potential of the clean membrane is, the higher
is ∆ζ [31].
Fig. 40: Effect of pH on zeta potential of: a) clean membranes and b) fouled membranes [31]
3.2.4 Influence of pH on coagulation coupled with UF with respect to NOM removal
NOM character, molecular weight distribution, water pH, ionic strength, and
membrane cut-off are the most important factors influencing NOM removal
by UF membrane. Higher removal efficiencies can be obtained by coagulation
pre-treatment.
Kabsch-Korbutowicz [32] assessed the influence of the pH on coagulation
coupled with UF in a lab scale study.
For this purpose, the pH of the feed solution was adjusted by adding
0.1 M NaOH or HCl to the range between 5 to 10. Two membranes, made of
polyethersulfone (PES) and regenerated cellulose (C), both with a MWCO of
30 kDa were tested. Alum was used as coagulant in different doses. To
determine the best pH value during pre-treatment, coagulation was
performed by the jar test method. Thereby the samples were rapidly mixed
for 3 minutes, afterwards they were stirred slowly for 30 minutes and at the
end, they were allowed to settle for 1 hour. Most of the NOM in the feed
solution came from aquatic origin with high hydrophobicity and of high MW
[32].

Fig. 41: Influence of alum dose and pH on
NOM removal efficiency by coagulation:
(a) colour removal, (b) abs 254 nm
decrease, (c) TOC removal. Coagulant
doses: D1, 1.795 g Al/m³; D2, 2.872 g
Al/m³; D3, 3.59 g Al/m³ [32]
As shown in Fig. 44 the removal of organic substances from the feed water
during coagulation was highly affected by the coagulant dose and the pH of
the solution. A higher pH caused a lower removal rate at given coagulant
dose. Kabsch-Korbutowicz concluded that the optimal pH for removal of
NOM is in the range of 5 to 6. The reason for this was the fact that the
ionisation of carboxyl groups of humic substances led to a condition in which
they had a negative charge. On the other hand, at pH conditions ≤ 6
aluminium formed substances with a positive charge, like Al3+ and Al(OH)2+.
These substances could either induce a complexation with humic substances
or they could neutralize the negatively charged sites of NOM (charge
neutralisation). At higher pH values, Al(OH)3 was predominant and the
NOM removal was dependent on the adsorption of humic substances on
Al(OH)3 crystals [32] (sweep coagulation).
The NOM removal efficiency of the membrane without coagulation was

dependent on the pH and on the membrane material. At low pH, NOM had a
smaller macromolecular configuration. This resulted in easier penetration
through the membrane. With increasing pH, the structure of these
macromolecules became more expanded, which was due to the dissociation
of carboxylic and phenolic groups of humic substances. Hence, NOM
separation was increased.
As pH increased the membrane pores became more negatively charged
because anions got beyond the plane of shear and gave the surface a negative
electro kinetic potential. The strong electrostatic repulsion between NOM and
the membrane pores improved the rejection of organic substances.
PES membranes had a better NOM separation efficiency than C membranes
because they were more hydrophobic and they had a denser structure.
However, the NOM removal was not satisfying if only the alum coagulation
or the UF were applied. The combined process of alum coagulation + UF

increased significantly the efficiency of NOM removal as can be seen in Fig.
42.
Fig. 42: Comparison of TOC removal in different processes (coagulant dose: 3.59 g Al/m³) [32]
For all the processes, the maximum efficiency of NOM removal was observed
at pH 6 with PES membranes and an alum dose of 3.59 g Al/m³ [32] In a
range between pH 6 to 8 similar TOC removal rates were observed.

4 Fouling control
4.1 NOM fouling
NOM membrane fouling depends on the interactions between the different

organics and inorganics as well as the individual and combined interactions
between the organics/inorganics and the membrane surface/pores. NOM can
be subdivided in particulate (P), colloidal (C) and dissolved organic carbon
(D).
Sundaramoorthy et al. [33] and Gimbel et al. [34] tried to determine which
NOM fraction is most responsible for irreversible fouling of submerged and
backwashed UF membranes with and without coagulation pre-treatment.
The particulate fraction was retained with a 0.45 µm flat sheet membrane run
below critical flux to achieve a sharp fractionation with minimal fouling. A
membrane with a MWCO of 5 kDa produced a filtrate containing colloidal
and genuinely dissolved NOM. Further fractionation in DOC (D) and COC
(C) was achieved with dialysis bags with a MWCO of 3.5 kDa. PACL was
used as coagulant at a concentration of 2.5 mg Al3+/L at pH 7.5. The PES
hollow fibre membranes had a nominal pore size of approximately 0.1 µm.
They were operated in the out-in mode. The five different NOM fraction were
tested for their fouling characteristics without (series 1) and with (series 2)
coagulation and the results are shown in Fig. 43a) to e). To compensate
changes in the starting point of pure water permeabilities and fluctuation of
water viscosity caused by temperature changes the results were plotted based
on normalised specific permeability (NSP %) vs. time (min).
Fig 43 a) shows, that the NSP decreased immediately after each backwash
(BW) because of a temporary release of blocked pores, which soon were
blocked again. In the case of pre-treatment of the P+C+D fraction with
coagulation, an improved membrane performance could be detected. This is
probably due to a better permeable fouling layer or to prevented pore
blockage. Regardless heavy fouling occurred. Fig 43 b) shows comparable
results for the C+D fraction, but the permeability of the fouling layer seemed
to be lower than in the P+C+D case. Fig 34 c) shows high losses of
permeability during each filtration interval of the P+C fraction but good
recovery though backwashing. Permeability was almost stable with
coagulation pre-treatment. Fig 43 d) shows that NSP declined significantly
during the first filtration cycle of the C fraction and gradually stabilized after
backwashing (BW). Coagulation did not advance the NSP considerably.
Hence, the coagulation impact on fouling in the C case is limited. The
membrane performance for the D fraction was very poor and BW showed no
effect when performed without coagulation (Fig 43 e). With coagulation, the
membrane performance was much better. This might be due to ligand effects
caused by coagulation, which changed the dissolved NOM physicochemical
characteristics.
To compare the NSP of the different fractions better, two factors were
introduced. The permeability decline coefficient (PDC) is defined as the

overall permeability decline during the filtration time. The coefficient of
influence of coagulation on the membrane performance (CIC) is defined as
the improvement in the membrane performance during the filtration of a
fraction with coagulation when compared to that without coagulation.
The importance and effectiveness of coagulation is emphasised by the fact
that the PDCs for all non-coagulated waters were about or higher than 0.1
whereas PDCs for coagulated waters varied between 0 and 0.07 (Fig. 44). It
stands out that those fractions containing particulates (P+C+D and P+C)
compared to fractions without particulates (C+D and C) added to
deteriorating fouling if not coagulated. However, if coagulation was
conducted the particulates were important to prevent colloidal fouling. The
worst fouling fractions were those containing colloids. All the fractions
caused severe fouling which could only be extenuated by coagulation in the
presence of particles. Genuine dissolved NOM showed the highest PDC
reduction when coagulation was conducted, changing from a high value to
close to zero for coagulated (D). The BW efficiency coefficient (BEC) is
introduced to compare the effect of BW on the different fractions. It is based
on the ability of pure water BW to re-establish the declining permeability to
its starting level. The mean BEC describes the BW efficiency throughout the
whole filtration time. If foulants cannot be removed by pure water or
permeate BW they are said to cause irreversible fouling. Fig. 45 also shows
the effect of coagulation on the mean BEC. The importance of the presence of
particulates during coagulation was highlighted again. BECs about 1.0 for the
fraction containing particles (P+C+D and P+C) with coagulation made BW
most efficient. On the other hand, coagulation had no influence on the fouling
mechanisms of colloidal NOM (C and C+D). Coagulation had its biggest
impact on dissolved NOM. Permeability decreased without coagulation even
during BW due to adsorptive fouling. In contrast, BEC was about 0.8 if
coagulation was conducted due to a transformation of the dissolved NOM
from highly adsorbing into non-adsorbing, detachable matter [33].

Fig. 43: Comparison of the NSP of the different fractions with (2) and without (1) coagulation pre-
treatment [33]
Fig. 44: Permeability decline coefficient (PDC) and influence of coagulation on membrane performance
[33]

Fig. 45: Mean backwash efficiency coefficients ( BEC) during filtration of NOM fractions and the
influence of coagulation on respective BECs [33]
All together, the fouling potential of the coagulated fractions could be

ordered as follows: (C) > (C+D) > (P+C+D) = (P+C) > (D). Particulates with
coagulation pre-treatment helped to minimise irreversible fouling.
Coagulation could not minimise the fouling caused by colloids, which is
considered the worst fouling.
The DOC fraction of NOM can be fractionated into hydrophobic, transphilic

and hydrophilic NOM fractions [33].
Kennedy et al. [35] investigated the rate of fouling and the fouling
reversibility of the isolated fractions. For this purpose, they used Liquid
Chromatography-Organic Carbon Detection (LC-OCD).
Experiments were conducted in lab scale with hollow fibre UF membranes
made of a hydrophilic PES/PVP blend with a lumen of 0.8 mm and a MWCO
of 150 – 200 kDa in the dead-end mode. The filtration mode was inside to
outside. NOM isolation was performed using XAD-8 and XAD-4 resins.
The feed water from Lake Ijssel contains very hydrophobic NOM (approx. 53-
55% hydrophobic NOM). Hydrophilic NOM (20-22%) and transphilic NOM
(25%) were almost alike. Surprisingly the specific UV absorbance (SUV254)
value of the hydrophobic fraction was lower than the SUV254 value of the
filtrate water and of the transphilic fraction. It was estimated to be higher
because it consisted mainly of aromatic compounds.
The transphilic fraction was expected to show a lower SUV254 value than the
hydrophobic NOM fraction because it was presumed to comprise more
hydrophilic NOM. The filtrate water should have comprised a mixture of all
NOM fractions and therefore have a lower SUV254 value than the
hydrophobic NOM fraction. This might be due to three different phenomena.

First, the aromaticity of the hydrophobic NOM fraction could have been
affected by the dilution of the hydrophobic and transphilic fraction prior to
the UVA254 measurement. This could result in a lower SUV254 value.
The LC-OCD analysis offered a second explanation. The hydrophobic NOM
fraction had a lower portion of humics and building blocks (46% in the case of
the hydrophobic NOM fraction) than the transphilic fraction and the filtered
water for 54% and 48%, respectively.
Third, the use of solvents and pH conditions necessary to bring about the
sorption/desorption of the compounds might have caused sample alteration.
Since the DOC rejection by the UF membrane was low (4.352 mg/L in the
feed water and 4.342 mg/L in the product water) they used chromatograms
of UF feed and product to inspect NOM fouling of the UF membrane.
As shown in Fig. 46 humics and building blocks (1 – 20 kDa) were hardly
rejected by the membrane (150 – 200 kDa) and therefore they did not
significantly contribute to the UF fouling. The UF membrane also rejected
only little amounts of LMW acids (LMW: low molecular weight) and neutrals.
Besides, LMW acids rejection was not likely because of the electrostatic
repulsion with the hydrophilic UF membrane. LMW neutrals (<0.35 kDa) can
readily adsorb on a negatively charged membrane surface or within the
pores, but they are so small that they were unlikely to be a major foulant. The
only group left to be responsible for the membrane fouling were the
polysaccharides (> 20 kDa). Polysaccharides in surface water originate from
algae and bacteria, e.g. from extracellular polymeric substances (EPS). They
were rejected due to size exclusion mechanism. The fouling layer was
described as sticky and difficult to be removed by backwashing.
Polysaccharides are neutral and therefore reduced the negative charge of the
UF membrane [35].
Fig. 46: LC-OCD analysis for feed and product water [35]

To gain a better understanding of the membrane fouling, four UF filtration
tests with four different types of feed water were performed using the same
flux. Fig. 47 shows that the highest fouling rate was observed for the
hydrophilic NOM fraction (0.0206 - 0.0255 bar/h). The rate increased about 12
to 24% in the first six-filtration cycles. The fouling rates of transphilic (0.0071
to 0.0064 bar/h) and hydrophobic NOM (0.0024 to 0.0032 bar/h) were by one
order of magnitude lower than the hydrophilic NOM and the filtered water.
UF membrane fouling rate was in the order: hydrophilic NOM > filtered
water > transphilic NOM > hydrophobic NOM .
Fig. 47: TMP vs. Time for each NOM fraction (138.5 L/m²·h) [35]
Fig. 48 shows a detailed analysis of the filtered water and the three NOM
fractions. As can be seen, only the hydrophilic and the filtered water
contained polysaccharides. This was the reason for the higher fouling rates of
these fractions.
The researchers also investigated the reversibility of the fouling for each
fraction.

Fig. 48: LC-OCD analysis for NOM fraction of Lake Ijssel water [35]
Colloidal matter was not expected to be significantly removed by the XAD-

8/4 columns and therefore it might be in the hydrophilic NOM fraction,
which is the effluent of the two-column array. This could be a reason for the
high fouling rates of this fraction. The colloidal matter was not efficiently
removed by backwashing and thus accumulated over time. Colloidal matter
and macromolecules were included in the polysaccharides (Fig. 48), which
were identified as the major foulant [35].
Another study by Kennedy et al. showed that the non-colloidal fraction of
NOM (< 1.3 nm), which comprised neutral amphiphilics, building blocks and
LMW polysaccharides, caused irreversible fouling. Polysaccharides were
removed by backwashing [36].
Lee et al. [37] also investigated NOM fouling. In their study they compared
four different membranes, two MF membranes with hydrophilic properties
(HPI) and two UF membranes, one with hydrophilic and one with
hydrophobic (HPO) properties. A contact angle of over 50° is considered as
hydrophobic. Tests were performed in a dead-end stirred cell filtration unit.
Taken the different water qualities and their fouling potential into
consideration, four different surface waters were selected. The waters were
pre-filtered with a 0.45 µm filter. After that, they were fractionated with XAD-
8/4 resins (Table 8).

Table 8: XAD -8/-4 fractionation of source (feed) water [37]
Source water Hydrophobic DOC [%] Transphilic DOC [%] Hydrophilic DOC [%]
Marne River 50 22 28
Cazau Lake 39 25 35
Bultière Reservoir 44 26 31
Yffiniac River 48 28 24
Permeation tests showed a greater flux decline for the Cazau Lake and
Bultière Reservoir waters, which contain a higher hydrophilic fraction than
for the other two waters. As in the tests by Kennedy et al. (2005) [35], organic
colloids and polysaccharides passed through the XAD 8/4 resins and ended
up in the hydrophilic fraction. SEC-DOC and UV responses of source waters
based on the relative MW distribution determined by PEG standards showed
a high first peak for these two waters. The first peak is typically assumed to
be proteins and/or polysaccharides. Flux decline trends of the different
membranes based on delivered DOC showed the most significant decline for
the hydrophobic MF membrane. UF membranes showed less flux decline
than MF membranes. Nevertheless, distinctive differences could not be
observed, suggesting that other membrane properties might be more
influential.
AFM and SEM analyses showed that the clean UF membranes had a
smoother surface than the MF membranes. The PES (UF-HPO) membrane
were smoothest and had the least flux decline for all the feed waters. Fig. 49
to Fig. 51 show the 3-D views, section analysis, and SEM images of clean and
fouled membranes, respectively. The fouled membrane surfaces appeared
smoother than the corresponding clean membrane surfaces and had a surface
coverage with a higher topography. AFM images supported the notion of
surface coverage as a fouling mechanism of UF membranes (Fig. 49). On the
other hand, the AFM images of MF membranes indicated that the filling of
the membrane pore structure with foulant material was the reason for
fouling, because the AFM “valleys” largely disappeared for the fouled
membranes (Fig. 50). The roughness of each membrane was very different.
Lee et al. concluded that the roughness could be more important in
membrane fouling by controlling interaction between fouling components
and the membrane surface / pores than the hydrophobic / hydrophilic
character of the membrane. Fig. 51 shows a reduction of the pores of the
GSWP (MF-HPI) membrane when filtered with Marne River water and pore
blockage with NOM material when filter with Cazau Lake water. This could
be due to the adsorption of NOM around membrane pores by smaller
molecules and/or pore blockage by larger molecules and colloids. This
showed the contribution of source water characteristics on membrane fouling.

Fig. 49: 3D views of UF membrane surfaces by AFM (membrane: YM100 (UF-HPI); from left: clean,
Cazau Lake and Bultière Reservoir[37]
Fig. 50: Section analysis of MF membrane surface by AFM (membrane: GVHP (MF-HPO); from left:
clean Cazau Lake and Bultière Reservoir) [37]
Fig. 51: SEM Images of GSWP (MF-HPI) membrane (from the left: clean and filtered with Marne River
and Cazau Lake; magnification: 9500 x) [37]
Contact angles were measured before and after filtration. At first, the contact
angle of hydrophilic membranes was less than 20° and it increased after
filtration. The contact angle of hydrophobic membranes was primarily greater
than 50° and it decreased after filtration. This reflected the character of the
foulant material. Backwash tests revealed that the flux recovery of UF
membranes was higher than that of MF membranes. This fact supports the
assumption that fouling of UF membranes was caused mainly by cake/gel
layer formation while MF membranes were affected more by the blocking of
pores.
Overall, they concluded that natural waters with a high content of
hydrophilic fraction resulted in more significant flux decline. This might be
due to colloidal and macromolecular matter in this fraction [37]. Later Lee et
al. [38] reported the same in another study. Membrane roughness was more

important with respect to flux decline than HPO/HPI of membranes. MF
membranes were more prone to NOM fouling than UF membranes.
4.2 Biofouling of UF membranes
Fouling caused by microorganisms is known as biofouling. It enhances the

fouling process by a formation of a biofilm on the membrane surface.
Biofouling is difficult to quantify because both the attachment of
microorganisms and their growth on the membrane surface have to be taken
into account. Different membrane surface properties show different
attachment behaviours for microorganisms. Since biofilms can exert a high
flow resistance, have a permeate contamination potential, are resistant against
disinfection, and may shield pathogens, they are undesirable and must be
controlled [39].
Hörsch et al. [39] used the in-situ analysis by fluorescence in-situ
hybridization (FISH) to trace the role of bacteria in the primary and mature
fouling layer.
Tests were conducted with a laboratory-scale flat-channel test unit (FCTU).
The feed water was reservoir water with low hardness and a relatively high
specific UV absorbance (SUV254). Rapid sand filtration was used as pre-
treatment. The PES UF membrane had a MWCO of 1850 Da and filtration was
performed in the cross-flow mode at a constant TMP of 5 bar. During the
tests, permeate flux decreased to 86% after 5 days of operation. After that,
flux stayed constant for the rest of the 33-day experimental period. TOC
rejection increased from 74% to 80 - 85%. Fig. 52 shows the formation of a
thick fouling layer on the UF membrane surface with pore blockage. This
layer might be due to mineral particles and algae, which were not retained by
rapid sand filtration. Measurements of the ratios of the different cations to the
TOC content of the fouling layers showed that NOM played an important
role in the layer formation. To highlight the bacterial role in the formation of
the fouling layer they used fluorescently labelled oligonucleotides specific for
α-, β- and γ subclass of proteobacteria. After a washing step, the sample was
incubated with a DAPI solution (4´6-diaidino-2-phenylindoldihydrochloride,
1 mg/L in phosphate buffered saline) for 10 minutes for the staining of all
cells. Fig. 53 shows that most of the DAPI-stained cells were γ-proteobacteria.
Less β-proteobacteria were found and only a few α-proteobacteria were
present. At the end of the 33-day experimental period, the bacterial
composition changed significantly. The number of γ-proteobacteria clearly
decreased, whereas α-proteobacteria and β-proteobacteria represented the
majority of the DAPI-stained cells. The fouling layer was much thicker and
consisted of bacterial cells, which were embedded in the matrix, NOM,
particles, and extracelluar polymeric substances released by the
microorganisms. Therefore, the fluorescence signals were more blurred. It
was assumed that the change in the bacterial composition resulted from a
different attachment behaviour of different microorganisms. To determine
which species were present in the raw water, the filtration was performed in
the dead-end mode to reject all bacteria. FISH analysis showed the same
bacterial composition in the raw water and in the 33-day mature biofilm.
From this, it can be concluded that the γ-proteobacteria were able to form a

primary biofilm on the membrane surface where the other proteobacteria
could attach and the growth of bacteria played a minor role in the biofouling
process. No influence of membrane properties on the formation of a biofilm
was found. Proliferation and selection of other species, which were not
included in this study, cannot be ruled out [39].
Fig. 52: SEM of the UF membrane, (a) cross-section of the new, unfouled membrane, (b) cross-section of
the membrane with fouling layer after 33 d of operation, arrow indicates the surface of the active layer,
(c) top-view with deposited particles after 33 d of operation [39]
Fig. 53: FISH of the UF fouling layer after 5 days of operation. (a) DAPI (total cell count), (b) α-subclass
(ALF1b, Fluos), (c) β-subclass (BET42a, Cy3), (d) γ-subclass (GAM42a, Cy5) [39]

4.3 Heterogeneous fouling in dead-end UF
Fouling is, most of the time, defined as the homogenous accumulation of

certain feed components on the membrane surface or within the membrane
pores [40]. Heijman et al. [40] investigated in a lab-scale test whether there is
any heterogeneous fouling in the dead-end UF if the hydraulic cleaning with
backwash and/or forward flush is not capable of removing all the cake
fouling or pore blocking in the membrane module.
For this purpose, they used PES membranes with a MWCO of 150-200 kDa
under constant flux condition with cyclic backwashing. They found out that
under constant flux, the resistance of the cake layer increased with every
filtration cycle. This was due to a decreased filtration area because the feed
solution was constant during all the filtration cycles. The backwash could not
remove all the fouling from the membrane and left some patches on the
surface. In the next filtration cycle, the cake was build up on a smaller
membrane area. This resulted in an increase of flux on the remaining
membrane area, which led to a faster cake build-up.
In another experiment with synthetic water containing iron hydroxide flocs,
the TMP was restored to the original level of a clean membrane. This was
done to indicate that the backwash (BW) was able to remove all solids from
the membrane surface. Surprisingly the forward flush pressure (FFP)
increased during the first six cycles enormously from 40 to 470 mbar and
stayed constant during the rest of the test. They observed that this was due to
the blocking of capillaries in the potting of the module. The membrane in the
potting was not contributing to permeation. This part of the membrane
neither contributed to the resistance of a clean membrane nor did it influence
the TMP. Fig. 54 shows the fouled membranes after a hydraulic cleaning. On
the brine side and the feed side, a significant number of capillaries were
blocked. After a chemical cleaning, fouling was only observed on the rear end
of the capillaries. Fig. 55 explains the reason why the fouling did not
influence the TMP. The capillaries were not affected by the blockage on the
brine side during filtration. Capillaries blocked on the feed side had to be fed
through the concentrate header. Feed water flew through the open capillaries
to the concentrate header, and from there to the blocked capillaries. That is
why blocking on both ends did not influence the TMP.
Fig. 54: Pictures are taken after a run of 18 h. The run was stopped after a hydraulic cleaning. The
blocking of the capillaries is both observed on the feed side (left) as well as on the concentrate side (right)
of the module [40]

Fig. 55: Schematic drawing of a module with blocked capillaries during filtration. The feed side of the
module is pressurized while the concentrate side is closed [40]

5 Cleaning procedure for UF membranes
5.1 Hydraulical cleaning of UF membranes
5.1.1 Air sparging in UF hollow fibres
The injection of air during a filtration or cleaning phase, in order to limit the
formation of a particle deposit or concentration polarisation, is known as air
sparging. It was first used in 1986 by Hitachi in electro dialysis systems [41].
Cabassud et al. [41] investigated the effect of air sparging in their lab-scale
study in an inside-out UF of hollow fibres to prevent particulate fouling. The
mean pore diameter was 0.01 µm and the membrane inner diameter was 0.93
mm. Air was added to the feed water at the bottom of the vertical module
through a porous membrane. The up-flow velocity of the raw water and the
air was constant. TMP was constant as well. ULS (liquid slug velocity) was
between 0.5 and 0.9 m·s-1 and UGS (gas slug velocity) was between 0 and 1 m·s-
1. The first test was conducted with river water and a clay suspension. It
revealed that air sparging was more efficient with water containing a high
fouling ability in terms of external particle deposit or of concentration
polarisation. The reduction of the hydraulic resistance by air increased with
the fouling ability of water and therefore with decreasing critical flux. Fig. 56
shows the results of a cake filtration modelling for the two-phase flow.
Fig. 56: Influence of gas velocity on cake porosity(a), specific resistance (b) and thickness(c) –
(clay- calim = 1 g l-1, ULS = 0.9 ms-1, TMP = 1 bar, T= 20°C) [41]
The two-phase flow expanded the cake until a gas velocity of 0.35 m·s-1 was
reached. From there, the cake porosity was too high to have a physical
significance and no more cake deposit was observed because the cake
thickness reached the range of the inner radius of the hollow fibre. Even near
the membrane surface, the particles were in suspension and could not form a
cake layer. Without a cake layer there was no more additional resistance to
mass transfer, thus flux was enhanced. Further analysis demonstrated that
the flux enhancement was mainly related to mixing and turbulence created by

the bubbles in the liquid phase. The flux enhancement can be linked with
Rem, which is the mixture Reynolds number [43].
5.1.2 UF in the feed-and-bleed mode (cross-flow)

The feed-and-bleed mode is used to control water recovery and maintain a
steady-state operation of the membrane system. Therefore, a certain amount
of retentate is bled periodically or continuously from the membrane system.
The amount, which is bled depends on the amount of permeate produced.
The concentration of retained materials is constant after steady state is
reached. The ratio of the recycle stream to the feed stream depends on the
module performance in terms of necessary cross-flow velocity for cake layer
control and possible flux. Choi et al [42] tried to further investigate this mode
in a pilot plant. Filtration was conducted with a polysulfone membrane with
a MWCO of 20 kDa with a pure water flux of 300 L/m²/h and 1 bar of TMP.
500 L of retentate were bled discontinuously after every 4-hour filtration cycle
for 1 min to reduce the concentration of retained materials in the loop. Fig. 57
shows the development of permeate flux over time. There was a decline in
permeate flux (X) at the end of each cycle which was assumedly caused by a
supply of cold fresh water which compensated the bled retentate. The
decrease in retentate concentration led to an increase in permeate flux (Y).
Thus, permeate flux decline during a 4 hour cycle was mainly caused by
concentration of retained matter, which is considered as reversible fouling.
The increasing back-diffusion of retained materials after bleeding caused a
disturbance of the concentration polarisation layer and a reduction of
concentration polarisation. Afterwards permeation decreased again because
of fouling and increasing retentate concentration (Z). The development of
permeate flux during feed-and-bleed mode was very similar to that of
membrane systems with periodic backwashing. Fig. 57 also shows how the
difference between maximum and minimum permeate flux during one cycle
was composed of Fn-fouling and concentration polarisation (Cn) [42].
Fig. 57: Conceptual diagram of permeate flux behaviour before and after bleeding [42]
At the beginning of the filtration experiment, bleeding of highly concentrated

retentate caused a significant increase of about 20% in the permeate flux.
However, over a long period of operation, the change in concentration of
retained materials in the loop before and after bleeding was so small that the
increase in permeate flux after bleeding was less than 2%.

During the 4000 hours of operation, permeate flux changed in three steps.
Within the first 1250 hours, permeate flux decreased sharply from 120
L/m²/h to 30 L/m³/h due to pore blocking and a rapid building of a fouling
layer. After that, permeate flux decrease gradually to 15 L/m²/h in 2800h
until a steady state condition was reached, were attachment of foulants onto
the membrane surface and their detachment due to tangential share was
balanced.
The permeate quality pertaining to turbidity, suspended solid, UV260 and
DOC was stable regardless of concentrating or diluting the retentate in each
cycle and fouling for long-term operation [42].
5.2 Chemical cleaning of UF membranes
Chemical cleaning of UF membranes is done in two ways. The first one is

known as chemically enhanced backwash (CEB), which is carried out to aid
the regular backwash process to stabilize the operation. The second one is
performed to restore membrane permeability and is known as cleaning in
place (CIP) and cleaning out of place (COP), respectively. Acids, bases, and
oxidants such as H2O2 are used for CEB because they neither produce
harmful by-products nor increase the re-growth potential for permeate. For
COP / CIP, chlorinated agents or citric acids are used. Since the choice of the
chemical, which should be used, is dependent on water quality parameters
and on the membrane system as well as membrane material, it is inevitable to
know more about the interactions between foulant and cleaning agent,
foulant and membrane surface, the cleaning agent and membrane surface,
and foulants among each other. Process parameters like temperature and flow
characteristics can aid chemical cleaning. Strugholtz et al. [43] tried to
evaluate the benefit of different cleaning agents and temperature influences
on the reduction of fouling. For this purpose, they extracted capillary
membranes from a submerged Puron® pilot plant in Roetgen (Germany),
which all showed the same amount of fouling. Table 9 shows the cleaning
conditions. Tests were conducted with a single capillary test unit. The
temperature of the cleaning agent was kept constantly at 20°C or 40°C. The
cleaning agent was circulated in the tube accompanied by air sparging for 2 h
to elute the fouling layer. Backwashing with the cleaning agent for 30 seconds
was conducted every 30 minutes to clean the pores of the membrane. After
that, the eluate was analyzed. The permeability of the capillary membrane
was also measured before and after the test. The permeability increase
coefficient (PIC) is used to describe the efficiency of cleaning [43].
Table 9: Cleaning conditions [43]
Cleaning agent Concentration pH-Value

NaOH 12
HCl 3
H2O2 250 ppm (unless it is stated otherwise)
NaOCl 50 ppm
Citric acid 2 g/L
“/NaOH”: cleaning at pH 12; “+”: successive cleaning steps

Fig. 58: Influence of cleaning agents on PIC [43]
The curve in Fig. 58 can be subdivided into four categories. Within the first
three categories the temperature showed no significant impact and the PIC
stayed almost constant at certain level. In the first category, there was almost
no change in PIC when cleaning was performed with H2O2 or distilled water.
The acids in category 2 reached a PIC of 1.5 whereas the oxidants, bases and
the combination of acid and alkaline cleaning in category 3 had a PIC of
approximately 2.5. The remarkable difference between neutral and alkaline
H2O2 stands out. This might be due to a more open structure of the fouling
layer at basic conditions that enabled a better cleaning with the agent. The
best results were achieved by a successive alkaline and acid cleaning at 40°C
and by H2O2/NaOH at 40°C. The order of basic and acid cleaning is
important because HCl followed by NaOH resulted in a lower PIC as the
other way round.
In order to know more about the influence of temperature on elution ability

and permeability, the cleaning regimes were sorted by characteristics and
compared with same compositions and rising temperature (Fig. 59).
Both inorganic and organic compounds were detached better at higher
temperature with all cleaners. NaOCl removed much more organics than
inorganics while HCl did not remove organics to a satisfying degree.
Oxidants were much stronger influenced by temperature in terms of
permeability recovery than acids and bases.

Fig. 59: Influence of temperature on elution ability and permeability [43]
After that, they focused on the cleaning efficiency of the agents on different
compounds. Inorganic compounds were poorly removed by uncharged
oxidants and H2O2 showed no effect at all. On the other hand, citric acid was
an effective agent for the elution of iron and formed complexes with iron.
Charged H2O2 followed by HCl was also successfully in iron and manganese
elution. The order of basic / acid cleaning steps showed an impact neither on
iron nor on aluminium dilution. However, NaOH followed by HCl showed
better results for manganese dilution as the other way round.
TOC can, as previously explained, be separated into hydrophilic, transphilic

and hydrophobic fractions. Strugholtz et al. subdivided it into hydrophobic
HOC, neutral, and hydrophilic CDOC (Fig. 60). Oxidants were a better
cleaning agent for hydrophilic compounds whereas a combination of base
and acid or NaOH at 40°C was more efficient for hydrophobic compounds.
The above average performance of hydrophobic OC removal by distilled
water at 40°C underlines the importance of temperature on the removal
efficiency of hydrophobic compounds. NaOCl and the combination of NaOH
followed by HCl was the best cleaning agent for organic compounds. HCl
itself was not suitable for membrane cleaning. The hydrophobic compound
was removed well with a base or with a combination with an acid. The
combination of NaOH + HCl at 40°C was better than at 20°C. For
HCl + NaOH no impact of temperature could be found [43].

Fig. 60: Impact of hydrophilic and hydrophobic components [43]
After that, the CDOC fraction was subdivided into polysaccharides, humic
substances, building blocks, neutral and amphiphile substances and acids
(Fig. 61).
Fig. 61: Fractionated CDOC [43]
Here, acidic cleaning showed almost no effect. NaOCl achieved the best
results among all the cleaning agents at a temperature of 40°C. Base and
combinations of base and acid showed good removal efficiencies. As
observed previously, the removal efficiency increased with increasing

temperature. Overall, a higher temperature improved the dissolution of
organic and inorganic compounds. A two-step cleaning in the sequence base
and acid showed the best overall performance. It can enhance a CEB notably,
because strongly fouling hydrophobic compounds can as well be removed as
inorganic colloids. Removal of organic compounds in CIP and COP can be
conducted with an oxidant such as NaOCl and inorganic compound removal
is best with a citric acid [43].

6 Case studies
As already described in chapter 1.3, the use of membranes in drinking water

production has rapidly increased. Table 10 shows a selection of installed or
planed ultrafiltration plants for drinking water production. The objective of
the last chapter is to show some examples of water treatment plants, where
ultrafiltration is already used as an alternative to conventional water
treatment.
Table 10: Overview of selected installed or planed UF plants in drinking water production
Location Membrane Source of raw Start-up Plant capacity Ref.

Supplier water [m3/d]
Canada (British Zenon Surface water - 160.106 Zenon
Columbia)
USA (California) Zenon Surface water - 94.625 Zenon
Canada (Ontario) Zenon Surface water under 261.165 Zenon
construction
USA (Wisconsin) Zenon Surface water under 189.250 Zenon
construction
Singapore Zenon Surface water under 181.699 Zenon
construction
Germany (Rehau) PALL Spring water 2005 3.120 PALL
Poland (Sucha PALL Surface water 2006 3.120 PALL
Beskidzka)
Germany PALL Spring water 2004 3.600 PALL
(Simmern)
USA (Menasha) Koch Surface water 2001 90.850 Koch
USA (Harrogate) Koch Spring water 1995 1135 Koch
Australia (Port Koch Surface water 2005 4920 Koch
Douglas)
Germany X-FLOW Surface water 2006 144.000 [44]
(Roetgen)
USA (Minnesota) X-FLOW Surface water 2005 265.000 [8]
United Kingdom X-FLOW Surface water 2002 34.439 [8]
(Inverness)
China INGE Surface water 2006 21.600 INGE
Switzerland INGE Surface water 2005 19.200 INGE
Germany INGE Spring water 2006 4.800 INGE
6.1 Roetgen (Germany
In Roetgen (Germany), one of the world’s largest UF plants started operation

in 2006. The plant has a treatment capacity of 6000 m³/h for drinking water
and a capacity of 600 m³/h for the treatment of the backwash water [44], [45].

The best position for an UF application was determined to be before the
existing conventional treatment. The membranes used for UF of the
coagulated raw water in the 12 membrane blocks with 42 pressure vessels in
each block are supplied by X-Flow (Fig. 63). In Roetgen, the water is first
taken from a reservoir and then stored in an intake tank. After that, the water
is pre-filtered to remove large particles, which might cause defects of
capillary membranes. PAC can be dosed if demanded. The pH value is
adjusted before coagulation by dosing either NaOH or CO2. Aluminium
sulphate or polyaluminium chloride is used as coagulant. Coagulation is
conducted in-line with a residence time longer than 1 minute. Permeate of the
second stage membrane (treatment of backwash water) is fed into the feed
water of the first stage membrane. Before permeate of the first stage
membrane reaches the limestone filtration, which removes residual iron and
manganese and where nitrification takes place, a significant hardening can be
achieved by dosing CO2. After that, residual CO2 can be removed with
NaOH. Before the storage tank, the water is prophylactically disinfected with
chlorine dioxide to prevent from re-infection in the distribution net (Fig. 62).
The microbiological removal efficiency of permeate is excellent (Fig. 66).
Turbidity, UV254 and TOC removal is efficient. Iron is completely removed
and the concentration is beneath the German drinking water regulation value
of 0.2 mg/L. The chemical enhance backwash (CEB) is carried out every 24
hours with caustic and acidic solutions [45]. Together with the second
membrane stage a total water recovery of 99 % can be reached. In the second
stage UF membranes from INGE are used. The specific costs for produced
drinking water with the extension of the existing WW Roetgen are presumed
to be below 10 euro cents/m³ [44]. The WW Roetgen started to produce
drinking water successfully at the beginning of 2006 [45].
Fig. 62: The new and advanced drinking water line of WW Roetgen [45]

Fig. 63: X-Flow membrane used at WW Roetgen
Fig. 64: Membrane modules at WW Roetgen
Fig. 65: Picture of WW Roetgen and draft design of the new drinking water line [46]

Fig. 66: Microbiological removal efficiency of WW Roetgen [45]
6.2 Hermeskeil (Germany)
The operational experience of the last 6 years from the UF drinking water
treatment plant at Hermeskeil (Germany) was published in 2005 by Hagen et
al. [47]. This system began to operate in 1999 and has a maximum drinking
water production capacity of 140 m³/h. The average capacity produced was
60 m³/h. The raw water had a pH of approximately 5.0 to 6.5. The iron
content in the raw water changed from season to season between 0.01 and
0.03 mg/L. Manganese content was between 0.02 and 0.08 mg/L. The
Hermeskeil treatment plant consists of two stages. In the first stage, the water
is pre-treated with a limestone filter for alkalisation and to adjust the
hardness as well as to remove manganese and aluminium. After that,
membrane filtration is conducted with hollow fibre membranes with an inner
diameter of 0.8 mm in the dead-end mode with an inside-out configuration.
During operation, different chemical cleaning methods were tested. Best
results with respect to TMP and permeability were achieved with a
combination of HCl and NaOH. This confirms the results by Strugholtz et al.
(2005) [43]. Turbidity removal was successful. Table 11 shows that bacteria
and protozoa are completely removed by the treatment plant.
Table 11: bacterial examination results [47]
Raw water Permeate

Giardia lamblia 6 in 120 L Not detectable
Cryptosporidium 4 in 120 L Not detectable
E. Coli [1/100 mL] 6 0
KBE 36 [1/mL]°C 29 0
KBE 20°C [1/mL] 262 0

Only 0.026% of the hollow fibres were damaged within 6.5 years of operation
and no membrane module had to be displaced for operational reasons. The
system was stable and reliable.
Operational costs were 11.9 euro cents/m³. They compose as follows:
Table 12: Total costs [47]
Base of costs €/m³

Amortisation Pumps and pipes 20 years 0.070
Energy 0.05 kWh/m³, 0.09 €/kWh 0.004
Attendance / manpower ½ h per working day 0.012
Chemicals HCl, NaOH 0.004
Membrane replacement 75 €/m²; endurance 7 years 0.025
Back wash water 6%; Raw water costs 0.14 €/m³ 0.004
Total cost: 0.119
Overall, the water treatment plant works stable, fully automated and safe.
The quality of the filtrate complies with the German drinking water
guideline.
6.3 Keldgate (UK)
Another operational experience is reported by Beforth [48]. The plant in

Keldgate (Great Britain) has a capacity of 3750 m³/h. Filtration was
conducted with a hollow fibre PES UF membrane with a MWCO of 150 kDa.
NaOCl, HCl and NaOH were used as chemicals for chemical cleaning. Their
focus was on the membrane integrity and on protozoa removal, especially
cryptosporidium. Integrity tests showed that the UF membranes obtained a
better performance than the required 4-log removal. No virus could be
detected in the permeate.
6.4 Switzerland
Another five UF treatment plants in the Switzerland have been used for the
production of drinking water for more than three years [49]. Their capacity
varies from 36 to 450 m³/h. The hollow fibre membrane modules are run in a
combined dead-end/cross-flow mode. Backwash is conducted every
30 minutes, disinfection one to three times a day, and chemical cleaning was
necessary between one to six times per year.
The water quality of permeates was good for all five plants. No bacteria were
detected and the turbidity was always below 0.01 FNU.
During the three years of operation, only four fibres were broken in more
than 200 modules. Raw water yields were between 93 and 98%. NaOCl was
used for disinfection and NaOH for chemical cleaning. Table 13 shows the
operational costs. Klahre et al. [49] conclude that UF with membranes is an
interesting alternative.

Table 13: Operating costs in four existing full-scale plants per cubic meter of permeate (electricity at
9 Cent €/kWh) [49]
Site Chemicals Energy Maintenance Module Total

[cent €/m³] [cent €/m³] [cent €/m³] replacement [cent [cent €/m³]
€/m³]
Thyon 0.005 0.5 1.5 1.5 3.5
Torgon 0.07 0.5 2.5 1.7 4.8
Vionnaz 0.07 0.7 1.7 1.6 4.1
Muotathal 0.07 0.4 0.9 1.6 3.0
mean 0.05 0.52 .65 1.6 3.85
6.5 Minneapolis (USA)
In Minneapolis (Minnesota, USA) the worldwide largest drinking water UF

plant with a capacity of 265 000 m3/d was installed. The raw water is
abstracted directly from the Mississippi River. The quality of the river water
is influenced by agriculture, power plant cooling and effluent from waste
water treatment plants. Table 14 gives an overview of the of the raw water
quality of the Mississippi River [8].
Table 14: Raw water quality of the Mississippi River [8]
Parameter Unit Average Maximum Minimum

pH - 8.3 8.9 7.7
Hardness mg/L as CaCO3 170 236 89
Temperature C° 11,7 30,7 0
Turbidity NTU 9,8 52,5 1,5
TOC mg/L 10 15 9
Colour CU 40 115 17
TDS mg/L 150 200 80
The UF plant is an extension of the conventional water treatment plant. Fig.

67 shows a process flow diagram of the conventional treatment plant and the
UF plant. PAC and potassium permanganate are added to the raw water.
Then the water is fed to a lime precipitator into which alum is also dosed.
Softened water is recarbonated in two tanks. One tank serves for the
conventional treatment plant and the other tank for the UF plant. After
recarbonation the water is treated by ferric chloride coagulation and
flocculation. Chlorine is also added for disinfection. Finally, the water is
applied to the UF treatment step [8].

Fig. 67: Process flow diagram for the water treatment plant [8}
The membrane units use UF membrane cartridges from X-Flow. Table 15

shows the characteristics of the installed X-Flow membranes [8].
Table 15: Characteristics of the X-Flow membranes [8]
Module model Xiga

No. of cartridges 4,032
Dimensions of cartridge 8 inch (200 mm) diameter x 60 inches (1,500
mm) long
Active membrane area (feed side) 377 ft2/cartridge (35 m2)
Pore size (µm) 0.02
Membrane material PES and poly vinyl pyrrolidone blend
Fiber flow configuration Inside-to-outside
Membrane hydrophobicity/hydrophilicity Hydrophilic
Maximum allowable operating pressure 45 psi (300 kPa)
Allowable operating pH range 2 to 12
Allowable cleaning pH range 1 to 12
Maximum allowable feed turbidity 5 to 7.5 NTU, but with unique conditions and
protocols, 15 NTU
Oxidant tolerance 500 mg/L as chlorine up to 40ºC, and up to
200 mg/L hydrogen peroxide at 40ºC
Permeate is used for backwashing the membrane units with backwash

intervals of 25 minutes. Chemical cleaning to restore permeability is only
used if required. It’s not being used routinely [8].
The following cleaning agents are used for chemical cleaning [8]:
• NaOCL (200 mg/L), as a 12.5 % solution

• NaHSO3 (300 mg/L), as a 38 % bisulphite solution, with 600 mg/L
hydrochloric acid as a 30 % solution
• Hydrochloric (800 mg/L), as a 30 % solution.

6.6 Choa Chu Kang (Singapore)
In Choa Chu Kang (Singapore) a submerged ultrafiltration system will be

constructed for surface water treatment. The ultrafiltration will be integrated
in an existing water treatment plant. The capacity of the ultrafiltration step is
about 180 000 m3/d. The aim of integrating UF is to improve treated water
quality. Following goals for the treated water are required [8]:
• The completion of the World Health Organisation (WHO) Guideline

Values for Drinking Water Quality
• Be free from algae
• Be free from waterborne organisms that do not fall into the traditional
microorganism categories
• Minimal DOC concentration
• Prolonged disinfection by using chloramines
Fig. 68 shows the process flow diagram of the water treatment plant in Choa
Chu Kang. The existing treatment includes aeration, pre-chlorination for
disinfection and algae control, and coagulation with alum and a coagulant aid
polymer. The submerged UF membranes, which are manufactured by
ZENON, will be integrated into an existing sand filter bed.
After the membrane step the water will be ozonated for disinfection, before it
passes to a granular activated carbon (PAC) contactor, which will be used for
DOC removal to improve the water stability. The last treatment steps are
chlorination followed by CO2 dosing, lime addition for corrosion control, and
ammonia addition to convert chlorine to chloramines [8].
Fig. 68: Process flow diagram for the water treatment plant [8]

Table 16 shows a summery of the Choa Chu Kang water treatment plant.
Table 16: Summary of the Choa Chu Kang water treatment plant [8]
Status of project Construction in 2006-2007

Capacity 181 699 m³/d (48 mgd)
Source water Surface (reservoirs)
Pre-treatment Alum coagulation, clarification
Type of membrane Zenon 1000
Design Flux 40 gfd; 68 lmh
Integrity testing Turbidity and particle counting
Main driver for integration Pathogen and algae removal
In 2000 a pilot plant was operated to investigate the capacity of the

ultrafiltration. For this pilot study two different membrane systems were
compared (ZENON and USFilter). The pilot plant includes pre-coagulation
with alum and PAC addition. Table 17 shows the pilot plant characteristics of
both membrane systems [8].
Table 17: Membrane pilot plant characteristics [8]
Parameter Zenon USFilter

Flow rate 3 m3/h 1.7 m3/h
Pore size 0.04 µm 0.2 µm
BW Frequency 20 minutes 30 minutes
TMP 0.17 to 0.61 bar 0.17 to 0.61 bar
BW duration 30 s 30 s
Following results could be demonstrated [8]:
• Reduction of the DOC concentration to about 2 mg/L

• DOC removal could be enhanced by PAC addition
• Enhanced coagulation process with increasing DOC removal
• Ability of immersed membranes to completely remove algae and
waterborne organisms that do not fall into the traditional
microorganism categories from the raw water
6.7 Iverness (UK)
In Inverness (UK) ultrafiltration is used for surface water treatment. The raw
water is abstracted from two lakes. Most of the catchment area is forest or
pasture. In the pasture some sheep and deer are grazing. So the risk of
Cryptosporidium contamination is elevated. Table 18 shows the raw water
quality of the Inverness water treatment plant [8].

Table 18: Feed water quality to the Inverness water treatment plant [8}
Parameter Units Amount of Min. Average Max.

Samples
pH 10 7.1 7.6 8.9
Alkalinity as CaCO3 mg/L 1 - 17.1 -
Hardness as CaCO3 mg/L 1 - 7.8 -
Temperature °C 8 3 10.1 17.2
Turbidity NTU 10 <0.06 0.36 0.73
1 - 2.4 -
Colour Hazen 10 3 5.8 9
Ammonia mg/L 10 <0.02 <0.021 0.03
Nitrate mg/L 10 <0.3 <0.65 1.0
Chloride mg/L 1 - 7.6 -
Sulphate mg/L 1 - 3.5 -
Iron mg/L 48 0.011 0.041 0.148
Manganese mg/L 10 0.011 0.005 0.013
E. Coli No./L 94 0 - 0
Total coli forms No./L 94 0 - 1
Plate counts. 22°C 93 0 - >10 000
Plate counts. 22°C 94 0 - 350
The ultrafiltration, which is installed, has a capacity of 34 439 m3/d. The start-
up of the plant was in 2002. The process flow diagram is shown in Fig. 69. The
raw water is pumped from the lakes to 80 µm rotating drum strainers. For
pre-coagulation PACL is used to remove colour from the water. The pH-level
for the coagulation process is 6.7. The installed membranes are ultrafiltration
membranes from X-Flow.
Fig. 69: Process flow diagram for the water treatment plant [8]

The water treatment plant includes seven primary treatment membrane units
and two secondary units for backwash water. Each primary membrane unit
has a membrane area of 2 940 m2. The membrane warranty of primary and
secondary units is seven years. The permeate of the secondary ultrafiltration
unit is combined with the permeate of the primary ultrafiltration unit. The
final treatment steps are lime addition, chlorination, phosphoric acid and
ammonia addition. The backwashing of the primary and secondary
membrane units are carried out every 40 minutes with duration of 45
seconds. For chemical backwashing hypochlorite with about 200 mg/L Cl2
followed by 400 mg/L NaOH is used [8].
Table 19 shows a summery of the water treatment plant in Inverness.
Table 19: Summary of the Inverness water treatment plant [8]
Status of the project Start-up in 2002

Capacity 34.439 m3/d
Pre-treatment PACL coagulation (pH 6.1), flocculation
Source water Surface water (lakes)
Type of membranes Norit X-Flow UF
Design flux 41 gdf; 69 lmh
Integrity testing Particle counter
Main driver for integration Cryptosporidium removal

7 Conclusions
Many studies on ultrafiltration membranes in drinking water production

have been conducted or are currently in progress with the intention to
improve the performance of this process. This report ought to give a
summary of these studies and deals with pre-treatment options, membrane
types, as well as process and water parameters, membrane fouling,
membrane cleaning procedures and operational experiences with UF
membranes.
Different methods of pre-treatment can be used before ultrafiltration.

Coagulation coupled with ultrafiltration is one of the most promising
drinking water production processes. Regarding removal rates and residual
aluminium, aluminium sulphate and polyaluminium chloride are better
coagulants than sodium aluminate. Iron chloride is a more efficient coagulant
than aluminium sulphate. A pH around 6 is recommended during
coagulation.
During in-line coagulation, under-dose conditions with acidic pH show the

best performance because it is possible to obtain good removal rates of
contaminants and improve physical performance. Nevertheless, ordinary
coagulation is superior to in-line coagulation. Dynamic membranes are a
promising alternative to current techniques used in drinking water
production, because tests show that they perform better than membranes
with standard or in-line coagulation as a pre-treatment. Metal membranes
have a potential for drinking water production, if the production costs can be
reduced. Absolute values of pH and coagulant dose depend on the nature of
the raw water and on the operational requirements.
Ultrafiltration membranes are a reliable barrier against bacterial, protozoa

and viruses. Coupled with coagulation LRVs (log reduction value) of 6.7 can
be obtained. This makes them suitable for water disinfection.
Test on the effect of ionic strength on humic substances removal show that
solutions with a low ionic strength have a higher permeability than solutions
with a high ionic strength. An increase in ionic strength neutralizes the
negative surface charge of the membrane and reduces the charge repulsion of
functional groups in the pores.
An improved removal of humic acids can be achieved if fibres with an
additive are used for filtration. Fibers spun under an air gap had both higher
flux and higher retention than wet spun fibres.
NOM causes membrane fouling. It can be subdivided in particulate (P).

colloidal (C) and dissolved organic carbon (D). The fouling potential of the
coagulated fractions can be ordered as follows: (C) > (C+D) > (P+C+D) =
(P+C) > (D). Particulates with coagulation pre-treatment help to minimise
irreversible fouling. Coagulation cannot minimise the fouling caused by
colloids, which is considered the worst type of fouling.

The dissolved organic carbon fraction of NOM can be fractionated into
hydrophobic. transphilic and hydrophilic NOM fractions. UF membrane
fouling is in the order: hydrophilic NOM > filtered water > transphilic NOM
> hydrophobic NOM. The difficulty of removal by backwashing can be
summarized as follows: hydrophilic NOM > transphilic NOM > hydrophobic
NOM. Polysaccharides are the major foulant. They might be in the
hydrophilic NOM fraction because they are not expected to be significantly
removed by the XAD-8/4 columns, which are used for the fractionation.
Biofouling is another form of fouling. It occurs in two steps. At first, a

primary biofilm is build up on the membrane. After that, other proteobacteria
can attach to them and build a fouling layer. Growth of bacteria plays only a
minor role in the biofouling process.
Chemical cleaning is used to restore the membrane permeability. A higher

temperature during the cleaning improves the dissolution of organic and
inorganic compounds. A two-step cleaning in the sequence base and acid
shows the best overall performance. It can enhance a chemical enhanced
backwash (CEB) notably, because strongly fouling hydrophobic compounds
can as well be removed as inorganic colloids. Removal of organic compounds
in cleaning in place (CIP) and cleaning out of place (COP) can be conducted
with an oxidant such as NaOCl and inorganic compound removal is best with
a citric acid.
Instead of dosing a coagulant before UF, the adsorption with iron oxide
particles is also an option for pre-treatment. Pre-chlorination is not efficient.
Ozonation with a minimum concentration of 0.05 mg/L of ozone
permanently in permeate can also prevent fouling efficiently and yields of
almost 100% can be obtained. Bromide in the raw water limits this process
because toxic bromates can be generated as oxidation by-products.
The WW Roetgen (Germany) and other drinking water production plants use
UF membranes successfully. Permeate quality complies with the drinking
water guidelines and membrane durability is good.
A direct comparison of the results of the sources used is difficult because

different membrane materials, operational modes, experimental setups, and
raw waters were used.
Recapitulating, the report shows that ultrafiltration is a reliable technique for

drinking water production.

8 References
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systems on surface water. Leeuwarden. 6. Aachener Tagung
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[24] Fiksdal. L.. Leiknes. T. . The effect of coagulation with MF/UF membrane
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[25] Costa, A. R., Pinho. M. N., Effect of membrane pore size and solution
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[26] Gosh. K.. Schnitzer. M.. Macromolecular structures of humic substances.

Soil Sci. 129 (1980).
[27] Cornet, P., Diffusion of humic acid in dilute aqueous solutions. J. Colloid
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[28] Saravia, P., Der Einfluss von Ladung und Ionenstärke auf den
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[29] Domany, Z., Galambos, I., Humic substances removal from drinking water
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[30] Qin, J.-J., Oo, M. H., Hollow fibre ultrafiltration membranes with enhanced
flux for humic acid removal. Journal of Membrane Science 247 (2005).
[31] Soffer, Y., Gilron. J., Streaming potential and SEM-EDX study of UF
membranes fouled by colloidal iron. Desalination 146 (2002).
[32] Kabsch-Korbutowicz. M., Application of ultrafiltration integrated with

coagulation for improved NOM removal. Desalination 174 (2005).
[33] Sundaramoorthy. K., Brügger. A., Studies on the minimisation of NOM

fouling of MF/UF membranes with the help of a submerged „single“ capillary
membrane apparatus. Desalination 179 (2005).
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[36] Kennedy, M.D., Natural Organic Matter fouling of UF Membranes

Colloidal and Non-colloidal NOM fouling. 6. Aachener Tagung
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UF With Coagulant As Pre Filtration

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Techneau, 06.

Ultrafiltration with pre-coagulation

Ultrafiltration with pre-coagulation

This report is:

3 Removal capactiy and impact of water quality parameters 32

Ultrafiltration with pre-coagulation in drinking water production – Literature review

Ultrafiltration with pre-coagulation in drinking water production – Literature review

In recent years, surface water purification with ultrafiltration membrane has

1.1 Requirements for water treatment

1.1.1 Surface water

The quality of surface water is determined by hydrodynamic, biological,

Ultrafiltration with pre-coagulation in drinking water production – Literature review

Fig. 1: Typical LC-OCD chromatogram of surface water [50]

The essential requirements to the treatment of the surface water are:

Normally the treatment of protected groundwater is less complex than the

Ultrafiltration with pre-coagulation in drinking water production – Literature review

1.2.1 Process description

Ultrafiltration (UF) is a pressure driven membrane process positioned

Particle size dP [µm]

Fig. 2: Classification of pressure driven membrane processes [6]

Ultrafiltration membranes are mainly made of polymers like polysulfone,

Fig. 3: Composition of an asymmetric membrane [6]

Ultrafiltration with pre-coagulation in drinking water production – Literature review

One of the major challenges in membrane filtration processes is to realise a

feed - raw water pF > pP permeate flux decline

permeate - filtrate time t

Fig. 4: Dead-end process [6]

constant feed pressure pF constant permeate flux vP

module flushing module flushing

filtration flushing filtration flushing

Fig. 5: Filtration intervals in dead end processes [6]

Ultrafiltration with pre-coagulation in drinking water production – Literature review

In order to apply sufficient permeate back-washing pressure a high stability

removal of fouling layer discharge of solids

Fig. 6: Module flushing concepts [6]

Ultrafiltration with pre-coagulation in drinking water production – Literature review

Fig. 7: Capillary module for dead-end operation [6]

Fig. 8: Cross-flow operation [6]

Ultrafiltration with pre-coagulation in drinking water production – Literature review

In submerged systems, membranes are dipped into tanks holding the

Submerged capillary module

Fig. 9: Submerged membrane system [6]

Ultrafiltration with pre-coagulation in drinking water production – Literature review

Irreversible cake layer

Inner pore adsorption

Fig. 10: Potential fouling mechanism [6]

In membrane processes chemical cleaning is very often used to clean the

• Support of the regular backwash (CEB – chemical enhanced

1.3 Use of ultrafiltration in drinking water production

Ultrafiltration with pre-coagulation in drinking water production – Literature review

Number of plants > 8 m³/h

Pre-treatment / Stabilisation Filtration / Hygienisation

Surface Drinking water

Filter backwash water

Ultrafiltration with pre-coagulation in drinking water production – Literature review

• disposal cost can be minimised by recycling the filter backwash water

1.4 Role of coagulation in combination with ultrafiltration in water treatment

In water treatment coagulation serves primarily to reduce turbidity. Further

Ultrafiltration with pre-coagulation in drinking water production – Literature review

(membrane) Filtration (membrane) Filtration (membrane) Filtration

The combination of the process shown in figure 13 depends from

The main objective of coagulation process is to aggregate small water

• Advanced removal of colloidal and suspended matters