Transcript

REVIEW ON THE FACTORS AFFECTING ULTRAFILTRATION HOLLOW

FIBER MEMBRANE OPERATIONAL PERFORMANCE IN WATER TREATMENT

Rosdianah Ramli1, Nurmin Bolong

1*, Abu Zahrim Yasser

2

1Nano Engineering and Materials Research Group (NEMs),

School Of Engineering and Information Technology, Universiti Malaysia Sabah, Jalan UMS, 88400 Kota

Kinabalu, Sabah. MALAYSIA 2Chemical Engineering Programme,

School Of Engineering and Information Technology, Universiti Malaysia Sabah, Jalan UMS, 88400 Kota

Kinabalu, Sabah. MALAYSIA

email: [email protected]; [email protected]

ABSTRACT. Ultrafiltration has been applied in the water treatment system since the last twenty

years. Among the membrane modules available, compact and self-supporting hollow fiber membrane

has been widely used as ultrafiltration membrane configuration. In this paper, the factors that have

influence on ultrafiltration hollow fiber membrane are reviewed. The highlight is on the operational

performance of the membrane. The factors are primarily membrane material, backwashing and pre-

treatment, as well as transmembrane pressure (TMP) and permeate flux. These factors are important

as points of reference when evaluating the operational performance of the ultrafiltration hollow fiber

membrane. Thus, enable appropriate and better judgement in selecting water treatment system.

Keywords- Water treatment, membrane processes, Ultrafiltration (UF), Hollow fiber membrane

INTRODUCTION

In membrane processes, the success of any separation system involving membrane depends on the

quality and suitability of the membrane incorporated in the system. Conventionally, water has been

treated primarily using physical-chemical treatment such as sand filtration, disinfection i.e.

chlorination and coagulation-flocculation via sedimentation process. Not only these conventional

methods required large area of operations that would require high operational cost, but may also be

incapable to treat several persistence pollutants (Kuch and Ballschmiter, 2001, Bolong et al, 2009a).

Membrane processes are becoming more popular in water treatment because the processes can

disinfect water without chemical additions and avoid the formation of toxic disinfection by-products

(Rana et al., 2005). Not only that, membrane technology has received more interest in recent years

due to stringent standard for water supply and effluent discharge. With its advantages such as small

operation area, high filtration efficiency as well as direct operational handling, membrane emerged as

a favourable filter media for water treatment system. However, the limitation such as membrane

fouling and operational life would be other factors to be considered. Further explanations of the

disadvantages were also discussed in the latter section of this paper.

The main configurations of polymeric membranes can be group as flat, spiral wound, tubular and

hollow fiber. Hollow fiber membrane configuration has the advantage of compact design with very

high membrane surface areas (Baker, 2004). Furthermore, hollow fiber configuration in water

treatment and reuse is favourable due to its large membrane area per unit volume of membrane

module. Hence, resulting in higher productivity, mechanically self-support which can be backwash for

liquid separation to provide good flexibility as well as easy handling during module fabrication and in

the operation (Chung et al., 2001). Many studies investigate on how to improve the filtration

behaviour of hollow fiber membranes to optimize its filtration performance. From many studies

conducted, it was found that the general filtration behaviour of hollow fiber membranes is

characterized by treatment operational such as time-dependent non-uniform distribution of

transmembrane pressure, flux, and filtration resistance along the fiber due to lumen-side pressure drop

induced by permeate flow (Chang et al., 2008). In choosing the right configuration for a water

treatment system, the module may be tested and evaluated first. For example, Groendijk and de Vries

(2009) tested three types of membrane configurations by evaluating the fouling behaviour of each

membrane before selecting the suitable membrane for their water treatment system.

It is understood that the membrane configuration would be the main important factors in most of these

work. However membrane performance in a complete water treatment system is also affected on the

operational and system design to achieve optimum operating condition. The optimal design

configuration of both affecting factors said at suitable operation is required to be evaluated as well,

which relies on the effective treatment (aiming for the required water quality/ contaminant removal)

and at the lowest overall cost. The issue of the ability in providing a system that moveable water

treatment which can be easily transported and relocated for off-site water treatment operation or

during water emergencies and may be extended for water reuse application especially at rural or

island users would be beneficial to be explored.

In spite of other type of membrane processes, this paper focuses on ultrafiltration membrane process.

Ultrafiltration has been recognized as one of the most applied process in water treatment system due

to its low pressure process thus requiring less energy and has less economic cost. Therefore, to

identify filtration performance from this process concentrating on the hollow fiber membrane

application, it is best to understand and analyse the factors that may affect the performance of the

ultrafiltration hollow fiber membrane; which is reviewed in this paper.

MEMBRANE PROCESSES

Membrane processes are categorized based on the driving force such as pressure (Drioli and

Macedonio, 2012), temperature and osmotic differences across the membrane (Mukiibi and Feathers,

2009; Fane et al., 2011; Peter-Varbanets et al., 2009). In the water treatment especially for drinking

water purposes, pressure-driven membranes are used (Bruggen et al., 2003). The pressure-driven

membranes are categorized into four classes according to the separation process, namely,

microfiltration (MF), ultrafiltration (UF), nanofiltration (NF) and reverse osmosis (RO). The two

former are low pressure processes (Guo et al., 2010) while the latters are high pressure processes.

Table 1 below summarized (Ozaki, 2004, Bruggen et al., 2003; Baker, 2004; Fane et al., 2008).).

Table 1 Classification of membrane processes in water separations

Particulars Microfiltration

(MF)

Ultrafiltration

(UF)

Nanofiltration

(NF)

Reverse Osmosis

(RO)

Pore size 10nm~1μm 3~10nm 2~5nm Not detectable

Retain

particulates

(MW)

>300,000 1,000~300,000 >150 <350

Applied pressure 0.005~0.2 MPa 0.01~0.3 MPa 0.3~1.5 MPa 1~10MPa

Main

applications

Removal of

particles and

bacteria, pre-

treatment for RO

and UF

Drinking water

production, fruit

juice clarification,

home water

purifiers

Removal of

micropollutants,

desalination of

brackish water,

concentration of

chemicals

Desalination of

brackish and

seawater.

Production of

ultrapure water.

Based on its contaminant removal efficiency, Mierzwa et al. (2008) had proven that UF membrane

has a high potential drinking water. This is statement has been supported by Guo et al. (2010) and

Peter-Varbanets et al. (2010).

ADVANTAGES & LIMITATIONS OF MEMBRANE PROCESSES

As mentioned previously, there are many advantages that favours membrane processes over the

conventional methods. The tabulated advantages and disadvantages of membrane processes are given

in Table 2.

Table 2 Advantages and Disadvantages of Membrane Process

Membrane process application Reference

Advantages Superior and consistent high quality permeate water

Capable of removing wider range of substances

Easy automation (operation) and maintenance

Less or no usage of chemicals

Much compacted system (33% less space occupied)

Low energy requirements (microfiltration and

ultrafiltration)

Nakatsuka et al., 1996;

Bodzek and Konieczny,

1998a; Rahman et al.,

2008;

Guo et al., 2009;

Rahman et al., 2012

Disadvantages Membrane fouling

Membrane integrity failure

chemical corrosion such as oxidation

faulty installation and maintenance

membrane stress and strain from operating

conditions, such as backwashing or excessive

movement due to vigorous bubbling

Damage by sharp objects not removed by pre-

treatment.

Nakatsuka et al., 1996;

Lenntech, 2011

Childress et al., (2005)

Guo et al. (2010)

The utmost limitation for membrane is fouling (Nakatsuka et al., 1996; Lenntech,2011). From the

Water and Wastewater Engineering book by Davis (2010), fouling is defined as the gradual decrease

in permeate water flux at constant pressure. While fouling is a problem for membrane processes

because it lessens the performance, thus the productivity of the membrane (Nicolaisen, 2002). Vos at

al. (1998) stated that fouling such as rapid fouling has causes unstable flux of the membrane to the

point that the water recovery to be less than 80%. Peter-Varbanets et al. (2010) mentioned how

fouling can occur; due to membrane adsorption (membrane hydrophobicity), pore blocking, cake

layer formation (Nicolaisen, 2002) and precipitation or biofilm formation (bio fouling). Nicolaisen

(2002) added particles in raw water as the fouling source.

Other limitation of membrane is membrane integrity failure. This is crucial for hollow fiber

membranes that are self-supporting. Childress et al. (2005) has given an example; when high pressure

is applied to a hollow fiber membrane with low modulus of elasticity, the fiber may break because it

is unable to withstand the pressure. All the advantages and disadvantages mentioned and discussed

above may also be dependent on the type of membrane configuration used in the system as shown in

Table 3 (Bolong, (2009b).

Table 3 Polymeric membrane configurations (advantages and disadvantages)

Configuration

(Area: Volume)

(m2 : m

3)

Packing Density Advantages Disadvantages

Plate and frame (also

known as flat sheet)

(400 – 600)

Moderate Can be dismantled for

cleaning

Complicated design

Cannot be backwash

and high cost

Spiral wound

(800 – 1,000)

High Low energy cost,

robust and compact,

low cost fabrication

Not easily cleaned –

cannot be backwashed,

poor handling solids

Tubular

(20 – 30)

Low Easily mechanically

cleaned, good solid

handling, tolerant of

high suspended solid

High capital and

membrane replacement

cost

Hollow fiber

(5,000 – 40,000)

Very high Can be backwashed,

compact design,

tolerant to high

colloidal levels

Sensitive to pressure

shocks

APPLICATION OF ULTRAFILTRATION MEMBRANE IN ‘MOVABLE’ WATER

TREATMENT SYSTEM

As mentioned in earlier section, ultrafiltration is has been recognized as one of the most applied

process in water treatment system. It provides an absolute barrier to particles, bacteria, high molecular

weight organic molecules, emulsified oils and colloids. Removal of chlorine-resistant pathogens and

their spores, such as Cryptosporidium from water supply is also possible (Kajitvichyanukul et al.,

2011).

Since the focus of this paper is primarily on ultrafiltration process, specifically on easily-transport

water treatment system; Table 4 simplifies several examples of applications of ultrafiltration

membrane in water treatment in the past years. Included is an inorganic (non-polymeric) membrane

which is ceramic. From the table, it can be seen that the efficiency of membrane ultrafiltration is very

good. From water treatment plant to portable water treatment device, the membrane filtration system

works properly and has high contaminants removal efficiency. Commercial portable water filters that

apply membrane as its filtering media are also included. These commercial portable water filters

(Katadyn Mini Ceramic, Sawyer PointONE™ Filterand LifeStraw®) have been regularly used and

received many good reviews from its users (eartheasy, 2011; thebackpacker.com, 2011; HikeLighter,

2012).

Table 4 Membrane application in water treatment (movable and easily transport) system

Types of water

treatment system

Membrane used Removal efficiency Reference

UF membrane filtration Cellulose acetate Hollow

fiber membrane

(MWCO >150kDa)

Turbidity: 100%

TOC: 100%

E. Coli: 100%

Fe: 98.9%

Mn: 77.8%

(Oe et al., 1996)

Katadyn Mini Ceramica 0.2 μm ceramic

Ag-impregnated

1.7 – 4.9 LRV* (Katadyn, 2011; Loo

et al., 2012)

Sawyer PointONE™

Filtera

U-shaped 0.1 Micron

Absolute Micron Hollow

Fiber Membrane

Protozoan parasites:

>99.99%

Bacteria: >99.99%

(Sawyer, 2005)

Mobile water maker 40 nm Ceramic Tubular Turbidity: >99.8%

TOC: 31.5%

E. Coli: >99.8%

Fe: >99.3%

Mn: >99.3%

(Groendijk and de

Vries, 2009)

Direct drinking water Thin Film Spiral wound

(MWCO 3.5 kDa)

Turbidity: 94.96%

TOC: 85.27%

E. Coli: 100%

Fe: 50%

Mn: 50%

(Mierzwa et al., 2008)

AQUAPOT Polyethersulfone (PES)

hollow fiber (MWCO

150 kDa),

Polysulfone (PS) spiral

wound (MWCO 100

kDa)

Turbidity: 53.6%

Total Coliforms: 100%

Thermotolerants

Coliforms: 100%

Colour(average): 39.5%

(Arnal et al., 2001);

(Arnal et al., 2008);

(Arnal et al., 2010)

LifeStraw®a 20 nm UF hollow fiber

membrane

Turbidity: 53.6%

E. Coli: 7.3 LRV

Cryptosporidium:

3.9 LRV

(VestergaardFrandsen,

2010)

Transportable UF

system

4 modules (18 m2) of

UF hollow fiber

(MWCO 100 kDa)

N/A (Barbot et al., 2009)

Enhanced Surface

Water Treatment Three 8 40” hollow

fiber membrane UF

modules

Turbidity: ~99.9%

Iron: ~99.9%

Phosphate: 66.7%

(Hofman et al., 1998)

UF for surface water Polyvinyl chloride

(PVC) hollow fiber

membrane

(MWCO 80 kDa)

Turbidity: 100%

Bacteria: 100%

Coliform: 100%

Natural Organic Matter:

20 – 40 %

(Guo et al., 2009)

a refers to commercial portable water filters that are available in the market.

LRV is log removal value

N/A: information not available

For UF water treatment application, hollow fiber is the most commonly used membrane configuration

(Kennedy et al., 2008) and it is also shown from Table 4. Furthermore, Mierzwa et al. (2008) found

that the required pressure for maintaining a certain flux for hollow fiber membrane is much lower

than that for spiral wound membrane.

FACTORS AFFECTING THE PERFORMANCE OF HOLLOW FIBER MEMBRANE IN

WATER TREATMENT SYSTEM

The performance of hollow fiber membrane as the filter media in water treatment system can be

influenced by several factors. Generally, the factors may be classified as shown in Figure 1 (Bolong,

(2009b)).

Figure 1 Factors influencing in membrane separation performance (adapted from: Bolong

2009a)

However in this paper, factors such as membrane material (polymer), permeate flux and

transmembrane pressure, pre-treatment of raw water before membrane filtration, backwashing and

chemical cleaning; were highlighted in this paper as they are the operating conditions that can be set

before the operation of membrane filtration system.

Factors influencing pollutants

separation in membrane process

Physical-chemical

properties of the

compound

Membrane properties

Membrane operating

conditions

• Molecular size

• Solubility

• Diffusivity

• Polarity

• Hydrophobicity

• Compound

• Permeability

• Pore size

• Hydrophobicity

• Surface charge

• Flux

• Transmembrane

pressure

• Rejections/recover

y

• Raw water quality

Membrane material (polymer)

Hollow fiber membranes mostly are made of polymeric materials due to ease of fabrication. UF

membranes are usually prepared by phase-inversion process and have an asymmetric porous structure

(Fane et al., 2008). Most common polymers used are cellulose acetate (CA), polysulfone (PS),

polyether sulfone (PES), polyvinylidenedifluoride (PVDF) and polyacrylonitrile (PAN) (Wagner,

2001; Fane et al., 2008). Choosing the right material is essential and dependent on the applications

and the operating conditions of the hollow fiber membrane. During the first decades of membrane,

CA was the main membrane material. But having low chemical and thermal stabilities as well as

narrow pH tolerance range had it substituted with other polymers (or sometimes polymer blends) to

produce UF membranes (Fane et al., 2008). These polymers such as PS and PVDF have wider range

of pH and resistant to temperature and chlorine attack.

Guo et al. (2009) used polyvinylchloride (PVC) as the polymer for the hollow fiber membrane that

was used in surface water treatment (as shown in Table 1). An advantage of PVC membrane is its

resistant to free chlorine compared to the common polysulfone membrane. This advantage is

important in terms of chemical cleaning because it can reduce membrane biofouling phenomena.

Nakatsuka et al. (1996) had shown in their study the comparison between two hollow fiber

membranes, same configuration but with different polymer. The study resulted on the CA membrane

had higher fouling resistance that PES membrane, thus making it easier to be backwashed. This was

due to the hydrophilic characteristic of CA membrane while PES membrane is hydrophobic.

Therefore, Nakatsuka et al. (1996) concluded that UF hollow fiber membrane water treatment

performance is strongly depending on the membrane polymer. This is supported by Bodzek and

Konieczny (1998b) that found that the removal efficiency of a membrane is depending on the

membrane’s polymer. This is because the hydrophobicity characteristic of the polymer will affect the

water contact between the membrane and the raw water. The higher the hydrophobicity of membrane,

the higher will the fouling tendency of the membrane is.

Therefore, membrane material (polymer or polymer blends) is important to determine the membrane

resistant to fouling. The membrane material will also determine whether the membrane can be

chemically clean by its range of chemical resistant characteristic or not.

Permeate flux and Transmembrane Pressure

According to Kennedy et al. (2008), membrane filtration system for water treatment can be operated

either in:

(a) constant permeate flux with varying pressure or

(b) constant transmembrane pressure with varying flux.

Permeate flux is the permeate flow rate per unit membrane area. While transmembrane pressure

(TMP) is the driving force for the flux.

In discussing the close relationship between permeate flux and transmembrane pressure (TMP), Xia et

al., (2004) stated that the permeate flux increases linearly with TMP when the TMP is less than

0.12MPa and up until the permeate flux is approximately 145 L/m2h. It is Darcy’s law region in which

the membrane permeability limits the permeate flux. The study found that the deviation from the

linear relationship is the UF region, where permeate flux did not depend on membrane resistance but

limited by the mass transfer condition in the boundary layer.

Since permeate flux is linear with TMP, the case can be vice versa as long as both are in the Darcy’s

law region. This is proven by a study conducted by Guo et al. (2009) where two constant permeate

fluxes which are 60 L/m2h and 100 L/m

2h were compared. The study shown that when the permeate

flux increases, TMP also increases. This is true, based on permeate flux-TMP relationship stated by

Xia et al. (2004) previously since the fluxes (60 L/m2h and 100 L/m

2h) are still in the Darcy’s law

region. However, there is an obvious difference in the increase of the TMP for both fluxes as observed

by Guo et al. (2009) in their study, where TMP for lower permeate flux (60 L/m2h) is much more

stable compared to that of the higher flux (100 L/m2h). The increase of TMP is not a very good

condition since it indicates increase of membrane fouling (Crozes et al., 1997; Guo et al., 2009).

Therefore Guo et al. (2009) concluded that the operation of higher constant permeate flux is less

stable compared to the lower one.

Permeate flux and transmembrane pressure (TMP) are correlated to each other. Either the membrane

filtration system is operated in constant permeate flux or constant TMP, it is recommended to keep

both in the Darcy’s law region i.e. permeate flux below 145 L/m2h or TMP below 0.12MPa. This is to

avoid membrane fouling, especially when the TMP is high.

Pre-treatment

In a membrane system, pre-treatment is recommended to control fouling (Guo et al., 2009). Pre-

treatment is optional to be added in any membrane filtration system since membrane processes are

able to treat water within a single operation (Bodzek and Konieczny, 1998). For the case of hollow

fiber membrane that can be automatically backwashed with permeate water, extensive pre-treatment

requirement reduces (Kennedy et al., 2008). However, it does not mean that pre-treatment is

absolutely not required in the membrane filtration system. Nicolaisen (2002) and Kennedy et al.

(2008) suggested that adequate pre-treatment of the raw water is mandatory for a well-functioning

membrane plant.

The effectiveness and necessity of the pre-treatment depends on the raw water quality. Most of the

time, pre-treatment as simple as sand filter is added to the water treatment system to filter large

particles and suspended solids. This action can actually help lengthening the membrane life because

large particles can cause damage to the membrane.

For UF membranes, it is good to have pre-treatment especially when the raw water contains

contaminant such as manganese. For example, Vos et al. (1998) reported that manganese in the raw

water could not be filtered by the UF hollow fiber membrane at first because it would change into its

ionic form, thus passing through UF. Then, Vos et al. (1998) modified their water treatment system

by adding pre-treatment before the UF unit. The pre-treatment chosen was oxidation by potassium

permanganate (KMnO4) where the manganese ions were oxidized. This pre-oxidation process

increases the manganese removal in the raw water by approximately 73%.

Guo et al.(2009) had shown the effects of pre-treatment to the hollow fiber membrane performance in

water treatment indicating that between the two membrane filtration systems performed; first with Y-

style filter (of 500 μm pore size) only and second with Y-style filter plus coagulation agents and bag-

style filter. The former only sieve contaminants’ particles that were larger than its pore size. However,

over the time, the retained particles form a cake layer thus causes clogging that reduces the permeate

flux. Furthermore, filtered particles (especially natural organic matter) can adhere to the internal

surfaces of the membrane which causes irreversible fouling. This is responded by sharp increase of

transmembrane pressure from 0.7 to 1.0 bar. On the other hand, when combined pre-treatment were

used, coagulation agents helped to combine those fine particles before entering the membrane and

then making it easier for the UF membrane to retain it.

Pre-treatment may be optional but it is still a big help to the membrane filtration system, especially

when the raw water contains large particles that could cause damage to the membrane.

Backwashing

It is been known that fouling is the major limitation for membrane. In order to overcome this

limitation, membrane will be backwash or clean between intervals during the filtration process

(Pervov et al., 1996; Hofman et al., 1998; Davis, 2010). The backwashing pressure will usually be

twice (Nakatsuka et al., 1996) or thrice (Hofman et al., 1998) the permeate flux. Backwash for hollow

fiber membrane can be carried out by changing the permeate water flow direction (Kennedy et al.,

2008). By that, the reverse flow washes out the foulants that formed cake layer on the membrane

surface during the filtration process.

The backwash interval between two filtration processes plays role in limiting the effect of fouling

during membrane filtration operation. In the study of drinking water treatment using ultrafiltration

hollow fiber membrane (Nakatsuka et al., 1996; Kennedy et al., 2008), it was found that the longer the

backwash interval, the more severe is the fouling. If consistently disregarded, the fouling can be

irreversible which would be much difficult to be removed.

The backwash frequency also plays an important role during the operation of membrane filtration

system in water treatment. Crozes et al. (1997) made a comparison of two backwash frequency on

membrane resistance to fouling. It was deduced that as the backwash frequency increases, TMP

increase can be reduced. As mentioned earlier, increase of TMP indicates the increase of fouling. So,

by reducing the increase of TMP in the filtration process, the membrane fouling can be reduced.

Backwash should not be rigid. It has to be adaptable to the raw water composition especially in the

period of rainfall (Hofman et al., 1998) when there will be rapid variations of contaminants. This is

because the concentration of contaminants in the raw water can affect the backwash efficiency.

Backwashing is essential for any membrane filtration system to avoid membrane fouling turning into

an irreversible fouling. In deciding the optimal conditions for backwashing, it is important to note the

backwash interval, backwash frequency and the raw water quality throughout the operation of the

membrane filtration system in the water treatment system.

Chemical cleaning

Backwash alone is not sufficient to remove fouling particles on the surface of the membrane.

Therefore, cleaning using chemicals that is more rigorous may be required (Davis, 2010). Chemical

cleaning can be applied to restore the membrane’s initial performance (Shengji et al., 2008; Chen et

al., 2008) and the increase of the reducing flux (due to fouling) after the cleaning indicates the

cleaning efficiency.

Oe et al. (1996) found that transmembrane pressure returned to its initial value and remained

unchanged after chemical cleaning of 5% citric acid solution circulated through the membrane module.

The chemicals used for the cleaning process depends on the raw water compositions. This is because

the chemical cleaning process must be able to remove the contaminants sticking on the membrane

surface that causes fouling. As mentioned in earlier section about membrane materials, it is important

to note the type of polymer that is used for the membrane. This is to avoid chemical attack such as

corrosion if the membrane polymer is not resistant enough to chemical.

Just like pre-treatment, chemical cleaning might be optional. But it is still a better option to have it

especially when the raw water quality is very low and backwashing is not sufficient to return

permeate flux or TMP.

CONCLUSIONS

The application of membrane processes in water treatment system particularly for easy-movable

system are getting more attention due to its advantages over conventional methods and is more

suitable for off-site water treatment operation or during water emergencies. It may also be extended

for water reuse application especially for rural or island users. For water treatment system such as

drinking water treatment, ultrafiltration hollow fiber membrane is a very good choice to be applied in

the water treatment. To get the most from the membrane operation, it is important to look into factors

that have influence on the membrane’s performance. As discussed in this review paper, membrane

material, permeate flux and transmembrane pressure (TMP) and backwashing are factors that can

affect the performance of ultrafiltration hollow fiber membrane in water treatment application. Pre-

treatment and chemical cleaning though optional can still be a great help to increase the filtration

performance of the membrane. The review is hoped to be beneficial in deciding the optimal

conditions for ultrafiltration hollow fiber membrane in water treatment system.

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