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Critical Reviews in Environmental Science and Technology


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Membrane Separation Bioreactors for Wastewater Treatment


C. Visvanathan , R. Ben Aim & K. Parameshwaran
a a b c

Environmental Engineering Program, Asian Institute of Technology, P.O. Box 4, Klong Luang, Pathumthani 12120, Thailand; Email: visu@ait.ac.th
b

Institute National des Sciences Appliques de Toulouse, Complexe Scientifique de, Rangueil 31077, Toulouse Cedex, France
c

3Center for Membrane Science and Technology, The University of New South Wales, Sydney 2052, Australia Published online: 03 Jun 2010.

To cite this article: C. Visvanathan , R. Ben Aim & K. Parameshwaran (2000): Membrane Separation Bioreactors for Wastewater Treatment, Critical Reviews in Environmental Science and Technology, 30:1, 1-48 To link to this article: http://dx.doi.org/10.1080/10643380091184165

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Critical Reviews in Environmental Science and Technology, 30(1):148 (2000)

Membrane Separation Bioreactors for Wastewater Treatment


C. Visvanathan,1 R. Ben Aim,2 and K. Parameshwaran 3
1Environmental Engineering Program, Asian Institute of Technology, P.O. Box 4, Klong Luang, Pathumthani 12120, Thailand; Email: visu@ait.ac.th; 2Institute National des Sciences Appliques de Toulouse, Complexe Scientifique de, Rangueil 31077, Toulouse Cedex, France; 3Center for Membrane Science and Technology, The University of New South Wales, Sydney 2052, Australia

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ABSTRACT: With continuing depletion of fresh water resources, focus has shifted more toward water recovery, reuse, and recycling, which require an extension of conventional wastewater treatment technologies. Downstream external factors like stricter compliance requirements for wastewater discharge, rising treatment costs, and spatial constraints necessitate renewed investigation of alternative technologies. Coupled with biological treatment processes, membrane technology has gained considerable attention due to its wide range of applicability and the performance characteristics of membrane systems that have been established by various investigations and innovations during the last decade. This article summarizes research efforts and presents a review of the how and why of their development and applications. The focus is on appraising and comparing technologies on the basis of their relative merits and demerits. Additional facts and figures, especially regarding process parameters and effluent quality, are used to evaluate primary findings on these technologies. Key factors such as loading rates, retention time, cross-flow velocities, membrane types, membrane fouling, and backwashing, etc. are some of the aspects covered. Membrane applications in various aerobic and anaerobic schemes are discussed at length. However, the emphasis is on the use of membranes as a solid/liquid separator, a key in achieving desired effluent quality. Further, technology development directions and possibilities are also explored. The review concludes with an economic assessment of the technologies because one of the key technology selection criteria is financial viability. KEY WORDS: membrane bioreactor, membrane technology, solid/liquid separation, membrane air diffusers, membrane fouling, backwashing, micro-porous membranes.

I. INTRODUCTION The use of biological treatment can be traced back to the late nineteenth century. By the 1930s, it was a standard method of wastewater treatment (Rittmann, 1987). Since then, both aerobic and anaerobic biological treatment methods have been commonly used to treat domestic and industrial wastewater. During the course of these processes, organic matter, mainly in soluble form, is converted into

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+, CH , NO , NO and biological cells. The end products differ H2O, CO2, NH4 4 2 3 depending on the presence or absence of oxygen. Nevertheless, biological cells are always an end product, although their quantity varies depending on whether it is an aerobic or anaerobic process. After removal of the soluble biodegradable matter in the biological process, any biomass formed must be separated from the liquid stream to produce the required effluent quality. A secondary settling tank is used for the solid/liquid separation and this clarification is often the limiting factor in effluent quality (Benefield and Randall, 1980). In recent years, effluent standards have become more stringent in an effort to preserve existing water resources. Recycling and reuse of wastewater for secondary purposes is on the rise due to dwindling natural resources, increasing water consumption, and the capacity limitations of existing water and wastewater conveyance systems. In both cases, achieving a high level of treatment efficiency is imperative. The quality of the final effluent from conventional biological treatment systems is highly dependent on the hydrodynamic conditions in the sedimentation tank and the settling characteristics of the sludge. Consequently, large volume sedimentation tanks offering several hours of residence time are required to obtain adequate solid/liquid separation (Fane et al., 1978). At the same time, close control of the biological treatment unit is necessary to avoid conditions that lead to poor settleability and/or bulking of sludge. Very often, however, economic constraints limit such options. Even with such controls, further treatment such as filtration, carbon adsorption, etc. are needed for most applications of wastewater reuse. Therefore, a solid/liquid separation method different from conventional methods is necessary. Application of membrane separation (micro- or ultrafiltration) techniques for biosolid separation can overcome the disadvantages of the sedimentation tank and biological treatment steps. The membrane offers a complete barrier to suspended solids and yields higher quality effluent. Although the concept of an activated sludge process coupled with ultrafiltration was commercialized in the late 1960s by Dorr-Oliver (Smith et al., 1969), the application has only recently started to attract serious attention (Figure 1), and there has been considerable development and application of membrane processes in combination with biological treatment over the last 10 years. This emerging technology, known as a membrane bioreactor (MBR), offers several advantages over the conventional processes currently available. These include excellent quality of treated water, which can be reused for industrial processes or for many secondary household purposes, small footprint size of the treatment plant, and reduced sludge production and better process reliability. The purpose of this monograph is to provide a comprehensive review of membrane bioreactor technology. The application of membranes in different stages of biological treatment processes, the historical development of membrane bioreators,

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FIGURE 1. Number of studies published on MBR.

and factors affecting the design and performance of MBR processes are discussed. A number of case studies for each type of major MBR application along with some cost information on MBR processes is also presented.

II. FEATURES OF MEMBRANE APPLICATION IN BIOLOGICAL WASTEWATER TREATMENT As our understanding of membrane technology grows, they are being applied to a wider range of industrial applications and are used in many new ways for wastewater treatment. Membrane applications for wastewater treatment can be grouped into three major categories (Figure 2): (1) biosolid separation, (2) biomass aeration, and (3) extraction of selected pollutants. Biosolid separation is, however, the most widely studied and has found full-scale applications in many countries (Table 1). Use of combined night-soil treatment and wastewater reclamation at plant scale operations in buildings in Japan are examples of some successful applications, and in these cases membrane-coupled technology is considered a standard process (Yamamoto and Urase, 1997). Solid/liquid separation bioreactors employ micro- or ultrafiltration modules for the retention of biomass for this purpose. The membranes can be placed in the external circuit of the bioreactor or they can be submerged directly into the bioreactor (Figure 2a). Asymmetric membranes consist of a very dense top layer or skin with a thickness of 0.1 to 0.5 m, supported by a thicker sublayer. The skin can be placed either on the outside or inside of the membrane, and this layer eventually defines the characterization of membrane separation.

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TABLE 1 Commercial Scale Solid/liquid Separation MBR Plants

Company Country Type of Waste Ref.

Commercial name Number of Plants Capacity (m3/d)

Rhone Poulenc-TechSep Dorr Oliver Thetfort Syst Kubota

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Mitsui Petrochemical Industries Zenon Env Inc. Dorr Oliver Membratek SITA/lyonnaise des Eaux Membratek Grantmij Degrement

UBIS MSTS Cycle-LET Kubota Kubota ASMEX Zenogem MARS ADUF

France USA USA Japan UK Japan Canada USA RSA France S.Africa Germany France Domestic Domestic Domestic Domestic Domestic Human excreta Industrial Industrial Industrial Landfill leachate Industrial Landfill leachate Industrial >40 1 >30 8 1 >40 1 1 2 3 2 3 1 <400 13.6 <200 10110 96 116 38 80/500 1050 100500 1050 500

Roullet, 1989 Smith et al., 1969 Irwin, 1990 Ishida et al., 1993 Brindle and Stephenson, 1997 Lambert, 1983 Knoblock et al., 1994 Li et al., 1984 Ross and Strohwald, 1994 Trouve et al., 1994a Brindle and Stephenson, 1997 Brindle and Stephenson, 1997 Brindle and Stephenson, 1997

A submerged membrane should be outer-skinned. In general, permeate is extracted by suction or, less commonly, by pressurizing the bioreactor. In the external circuit, the membrane can be either outer- or inner-skinned, and the permeate is extracted by circulating the mixed liquor at high pressure along the membrane surface. In the later case, the concentrated mixed liquor at the feed side is recycled back to the aeration tank.

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FIGURE 2. Features of membrane application in biological wastewater treatment. (B, bioreactor; M, membrane module; I, influent; E, effluent.) (Adapted from Brindle and Application in Wastewater Treatment.)

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Gas-permeable porous membranes can be used to aerate the mixed liquor in the aeration tank by bubbleless oxygen mass transfer (Yasuda and Lamaze, 1972). At the same time, they can be used for fine bubble aeration (Semmens, 1989; Matsuoka et al., 1992). In certain cases, the membrane can act as support for biofilm development, with direct oxygen transfer through the membrane wall in one direction and nutrient diffusion from the bulk liquid phases into the biofilm in the other direction (Brindle and Stephenson, 1996). Because the membranes can form bubble-free or fine-bubble mass transfer, the efficiency is very high. Conventional membrane modules can be used in either a flow-through or deadend mode as presented in Figure 2b. In the flow-through mode, the air or oxygen is continuously pumped through the hollow fibers and gas is vented to keep the partial pressure of oxygen high along the membrane. In the dead-end mode, the membrane is pressurized with air or oxygen by sealing one end of the fibers or by sending the gas from both ends. Most studies reported to date have focussed on the flow-through mode, and researchers argue that the dead-end mode should be avoided because it significantly reduces performance and may result in water vapor condensation inside the membrane fibers. However, because air or oxygen is vented out in the flow-through system, part of the pumped gas is wasted, and thus the gas transfer efficiency is reduced. In addition, volatile organic compounds (VOCs) can diffuse across the membrane into the air stream (Semmens, 1989), VOCs in wastewater can be very effectively stripped and vented off to the atmosphere. Both these problems can be overcome in the dead-end mode. Also, as the total amount of air/oxygen supplied should diffuse through the membrane module, the efficiency is improved and VOCs stripped off can be minimized if not completely reduced. An extractive membrane bioreactor was developed to extract (by dialysis) toxic organic pollutants present in industrial wastewater to a bio-medium for subsequent degradation (Livingston, 1994). In dialysis mode, organisms can be maintained in an optimal growth environment through nutrient supplementation while at the same time digesting inhibitory or recalcitrant compounds that diffuse across the membrane. Mass transfer of the pollutants across the membrane is driven by a concentration gradient, because the bio-medium passing on the membrane walls acts as a sink. Although these three applications are described separately, they are not mutually exclusive, and they may be coupled together to achieve added advantages for each process (Brindle and Stephenson, 1997). For example, a study by the authors to use hollow fiber membrane for solid/liquid separation and aeration in alternate cycles indicates such coupling (Parameshwaran et al., 1998).

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III. DEVELOPMENT OF MEMBRANE BIOREACTORS Membranes have been finding wide application in water and wastewater treatment ever since the early 1960s when Loeb and Sourirajan invented an
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asymmetric cellulose acetate membrane for reverse osmosis. Many combinations of membrane solid/liquid separators in biological treatment processes have been studied since. The trends that led to the development of todays MBR are depicted in Figure 3. When the need for wastewater reuse first arose, the conventional approach was to use advanced treatment processes (Figure 3a). For irrigation, this treatment may be limited to filtration and disinfection, whereas for building reuse or ground water recharge it may also include reverse osmosis (RO). For example, Water Factory 21 in Orange Country (California, USA) uses a treatment process that consists of lime softening, air stripping, recarbonation, sand filtration, carbon adsorption, and RO for biologically treated effluent (Mills, 1996). The treated water is used to recharge the ground water. This scheme is relatively complex and produces large amounts of chemical sludge. The progress of membrane manufacturing technology and its applications could lead to the eventual replacement of tertiary treatment steps by microfiltration or ultrafiltration and this simplified method is being evaluated at Water Factory 21 in the U.S. Parallel to this development, microfiltration or ultrafiltration was used for solid/liquid separation in the biological treatment process and the sedimenta-

FIGURE 3. Trends in MBR development.

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tion step could also be eliminated. By pumping the mixed liquor at a high pressure into the membrane unit, the permeate passes through the membrane and the concentrate is returned to the bioreactor (Hardt et al., 1970; Arika et al., 1977; Krauth and Staab, 1988; Muller et al., 1995). However, higher energy costs to maintain the crossflow velocity led to the next stage of development submerging the membranes in the reactor itself and withdrawing the treated water through membranes (Yamamoto et al., 1989; Kayawake et al., 1991; Chiemchaisiri et al., 1993; Visvanathan et al., 1997). In this development, membranes were suspended in the reactor above the air diffusers. The diffusers provided the oxygen necessary for treatment to take place and scour the surface of the membrane to remove deposited solids. In a parallel attempt to save energy in membrane coupled bioreactors, the use of jet aeration in the bioreactor has been investigated (Yamagiwa et al., 1991). The main feature is that the membrane module is incorporated into the liquid recirculation line for the formation of the liquid jet such that aeration and filtration can be accomplished with only one pump. Jet aeration works on the principle that a liquid jet, after passing through a gas layer, plunges into a liquid bath entraining a considerable amount of air. The limited amount of oxygen transfer possible with this technique restricts this process to small-scale applications. However, using only one pump makes it mechanically simpler and therefore useful to small communities. The invention of air back-washing techniques for membrane declogging led to the development of using the membrane itself as both clarifier and air diffuser (Parameshwaran et al., 1998). In this approach, two sets of membrane modules are submerged in the aeration tank. While the permeate is extracted through one set, the other is supplied with compressed air for backwashing. The cycle is repeated alternatively, and there is a continuous airflow into the aeration tank, which is sufficient to aerate the mixed liquor.

A. Advantages of MBR There are many advantages in using a MBR process, the prime ones being the treated water quality, the small footprint of the plant, and less sludge production and flexibility of operation.

1. Treated Water Quality


The major problem of conventional activated sludge processes is the settling of sludge. This is caused by poor flocculation of microfloras or the proliferation of filamentous bacteria. Because solids and colloids are totally eliminated through membrane separation, settlement has no effect on the quality of treated water. Consequently, the system is easy to operate and maintain. This is important with industrial wastewater, because a lack of nutrients leads to excessive growth of filamentous organisms resulting in poor settlement. Because the final effluent does
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not contain suspended matter, this enables the direct discharge of the final effluent into the surface water and the reuse of effluent for cooling, toilet flushing, lawn watering, or, with further polishing, as process water.

2. Flexibility in Operation
In a MBR, sludge retention time (SRT) can be controlled completely independently from hydraulic retention time (HRT). Therefore, a very long SRT can be maintained resulting in the complete retention of slow-growing microorganisms such as nitrifying or methanogenic bacteria and this results in greater flexibility of operation.
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3. Compact Plant Size


Volumetric capacities are typically high because a high sludge concentration can be maintained independently of settling qualities. HRTs as low as 2 h have been satisfactorily applied (Chaize and Huyard, 1991), and fluctuations on volumetric loading have no effect on the treated water quality (Chiemchaisri et al., 1993). For example, sludge concentrations between 25 and 30 kg/m3 have been achieved regularly as opposed to the more common 4 to 6 kg/m3 in the conventional aerobic process (Yamamoto and Win, 1991). Moreover, the higher turbulence maintained within the mixed liquor to prevent the membrane from fouling also prevents the flocculation of biosolids and keeps them highly dispersed. An analysis on the floc size distribution of MBR sludge and conventional activated sludge indicates that the floc size in the MBR (a number of samples from different MBR plants were analyzed) are very much smaller than 100 m and concentrated within a small range. On the other hand, floc size from conventional activated sludge processes varied from 0.5 to 1000 m (Zhang et al., 1997). The smaller flocs from MBRs could stimulate a higher oxygen and/or carbon substrate mass transfer and thus higher activity levels in the system. Zhang and co-workers (1997) also found that nitrification activities in MBR processes averaged 2.28 g NH4N/kg MLSS.h, which was greater than in conventional processes (0.95 g NH4N/kg MLSS.h). Also, there is an enormous saving in space with MBRs because there is no need for secondary settling devices and post-treatment to achieve reusable quality.

4. High Rate Decomposition


Treatment efficiency is also improved by preventing leakage of undecomposed polymer substances. If these polymer substances are biodegradable, they can be broken down with a reduction in the accumulation of substances within the
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treatment process. On the other hand, dissolved organic substances with low molecular weights, which cannot be eliminated by membrane separation alone, can be broken down and gasified by microorganisms or converted into polymers as constituents of bacterial cells, thereby raising the quality of the treated water. For example, the permeate from microfiltration of screened raw sewage (feed average BOD5 = 230 mg/l) had an average BOD5 of 93 mg/l. This was mainly the soluble portion of the influent BOD5, although it showed 99% removal of suspended solids and 5.8 log removal of fecal coliforms (Johnson et al., 1996). In contrast, most MBR studies indicate the effluent BOD5 is below 5 mg/l (Parameshwaran and Visvanathan, 1998; Buisson et al., 1997; Trouve et al., 1994). Due to the high biomass concentration and the fact that bio-oxidation is an exothermic process, temperature increase can be maintained at the maximum activity temperature level. Maximum growth rates are about five times higher than the activity commonly observed in activated sludge systems. Based on cubic meter of reactor volume, combining high activity with high biomass concentration results in conversion rates 10 to 15 times higher than conventional conversion rates (Buisson et al., 1997), an especially useful feature in cold climates.

5. Low Rate Sludge Production


Studies on MBR indicate that the sludge production rate is very low (Table 2). Chaize and Huyard (1991) have shown that for treatment of domestic wastewater, sludge production is greatly reduced if the age is between 50 and 100 days. Low F/M ratio and longer sludge age in the reactor is generally used to explain this low production rate. Praderie (1996) demonstrated that the viscosity of sludge increases with age, eventually limiting the oxygen transfer in the MBR system. Therefore, he recommends limiting the MLSS concentrate to 15 to 20 g/l for effective oxygen transfer. It was also noted that with increased age there was greater difficulty in sludge dewaterability, which could be attributed to excess amount of cellular polymer formation ( Parameshwaran, 1997; Erikson et al., 1992). It is also anticipated that micrological activity can be modified with increased sludge age, but little published information is available on the subject. The initial microscopic observation (Praderier, 1996; Pliankarn, 1996) on microorganism population indicates that with increased sludge age, reduction in filamentous bacteria increased rotifers and nematodes.

6. Disinfection and Odor Control


In this membrane filtration process, the removal of bacteria and viruses can be achieved without any chemical addition (Pouet et al., 1994; Langlais et al., 1992; Kolega et al., 1991). Because all the process equipment can be tightly closed, no odor dispersion occurs. Comparison of conventional biological processes and MBR is shown in Table 3 and depicts the advantages discussed above.
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TABLE 2 Comparison of Sludge Production in Conventional Activated Sludge Process (ASP) and MBR Process Treating Domestic Wastewater
Type of Process ASP ASP ASP MBR MBR MBR Sludge production 0.71 kg MLSS/kg BOD5 0.7 kg MLSS/kg BOD5 0.6 kg MLSS/kg BOD5 0.53 kg MLVSS/kg BOD5 0.26 kg SS/kg BOD5 0.22 kg MLSS/kg BOD5

SRT (d) 1020 14 33 25 25 50

Ref. Hsu and Wilson, 1992 E.I.A, 1994 E.I.A, 1994 Trouv et al., 1994a Trouv et al., 1994b Takeuchi et al., 1990

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With the exception of wastewater reuse, membrane separation activated sludge processes have not been widely used. Obstacles to more widespread use include: High capital and operating costs Current regulatory standards can be achieved by conventional treatment process Limited experience in use of membranes in these application areas Lack of interest by the membrane manufacturers

Membranes will only find greater application in the wastewater industry if they can achieve the required regulatory standards or better at the same or less cost
TABLE 3

Comparison of Operating Data for Conventional, Extended Aeration ASP, and AS/UF Treatment Processes
Processes ASP/UF Parameters System reactor volume Influent BOD System MLSS Organic loading rate Volumetric loading rate Reactor dissolved oxygen Sludge retention time Re-circulation ratio Hydraulic retention time From Smith et al., 1969. Unit 1 mg/l mg/l kg BOD/kg. MLSS.d kg BOD /m3.d mg/l d % h 2,663 250 10,000 0.12 1.35 1.50 Infinite 240 5 Conventional ASP 3,423 250 2,500 0.200.70 0.59 1.50 20 25 6 Extended aeration ASP 13,694 250 3,500 0.100.15 0.27 1.50 11 50100 1224

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compared with present processes, or if regulations were to tighten further such that conventional processes can no longer achieve the desired effluent quality.

IV. FACTORS AFFECTING THE MBR PROCESS PERFORMANCE The main aim of membrane-coupled bioreactors is to improve the efficiency of the biological process step such that high-quality effluent is obtained. Because biological treatment and membrane separation are rather distinct processes, the combined MBR process is relatively complex. To optimize the MBR process, many parameters have to be considered. These include solid concentrations, sludge age, and the hydraulic retention time (HRT) in the biological step as well as the flux rate, material costs, and the energy cost of the membrane separation. The treatment and disposal of the waste sludge also needs to be considered. Comparisons made on the waste sludge properties of the conventional activated sludge process and the MBR process indicates that dewatering of MBR waste sludge is difficult compared with the conventional process. This has been attributed to higher organic matter content and excess production of extracellular polymers (Parameshwaran, 1997). As all these parameters are interrelated, optimization is complicated. For example, an increase in sludge concentration can enhance the biological stage. However, when sludge concentration exceeds a certain limit, the permeation flux rapidly declines due to a dramatic rise in the viscosity of the sludge mixture (Praderie, 1996). An increase in sludge concentration can also affect the gas transfer efficiency, and the energy requirements for the aeration therefore increase will (Praderie, 1996). Permeation flux of membrane filtration is affected by the raw materials of the membrane and its pore size as well as operational conditions such as the pressure driving force, the liquid velocity/turbulence, and the physical properties of the mixed liquor being filtered (Tables 4 to 6). A. Type of Membrane Selection of the membrane module plays an important role on the membrane flux achieved. Membranes can be categorized according to the materials used (organic or ceramic), membrane type (microfiltration or ultrafiltration), module type (plate and frame or tubular or hollow fiber), filtration surface (inner skin or outer skin), as well as the module status (static or dynamic membranes). All are being tested and many combinations have been considered. There are, however, overlaps and omissions in the combinations considered largely due to poor communication among international researchers. The flux will vary depending on the combination considered. For example, submerged hollow fiber membrane modules (external skin) show the lowest flux of 3.5 l/m2.h, while ceramic microfilters show the highest of 100 l/m2.h (Tables 4 to 6). Smooth surface membranes (ceramic) offer more resistance to cake layer
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TABLE 4 Characteristics and Operating Conditions of Aerobic MBR Process (Membrane in External Circuit)
Domestic MF (hollow fiber) MF/UF (tubular) MF/UF 200,000 Ceramic 0.1 1.1 100 Synthetic UF (tubular)

Wastewater type

Membrane configuration

Membrane material

Pore size (Dalton/m) 266 0.42 1.5 100200 152186 15 Smith et al., 1969 1969 25 1/h Audic, 1986 20 810 1090b Chaize and Huyard, 1991 29 3.7 0.8 80100 Trouve et al., 1994c

UF (plate and frame) Noncellulose organic MF (hollow fiber) Polyvinyl acetate UF (plate and frame) Polysulfone/ cellulose 50,000 Polysulfone/ acrylic 0.1/50,000/ 800,000 15 150400 0.00385 2080 20

MF (hollow fiber) Polyester 0.1 2.23.6 200250 30 20 Bailey 1994

UF (spiral wound) Polysulfone/ 50,000 0.5 100

Polysulfone/ 0.01 0.1 4.5 135260

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20 540 Muller et al.,1995 4.811.4 Suwa et al., 1992 25 412 29.2 1/month Ishiguro, 1993 Industrial Sour vegetable canning Ice cream Tubular Ceramic 0.2 0.06 10 25 24 Scott and Smith, 1997 UF hollow fiber Organic 2 140 30 7.512.4 50 Hare et al., 1990 UF plate and frame Polysulfone 2.17 2 190390 3038 2028 2370 1/h Sato and Ishi, 1991 UF Tubular Polysulfone 0.04 0.22 2.53 275 31.5 11 66 Krauth and Stab, 1993 UF Tubular Polysulfone 0.01 0.551.1 250 47 40 Lbbecke et al., 1995

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Filtration area (m2) Cross flow velocity (m/s) Transmembrane pressure (kPa) Temperature (C) MLSSa (kg/m3) Flux (L/m2.h) Frequency of cleaning Reference

27 640 45 Lbbecke et al., 1995

Wastewater type

Membrane configuration

Membrane material Pore size (Dalton/m) Filtration area (m2) Cross flow velocity (m/s) Transmembrane pressure (kPa) Temperature (C) MLSSa (kg/m3) Flux (l/m2.h) Frequency of cleaning Reference

Mixed-liquor suspended solids. Unit (l/m2.h.bar).

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TABLE 5 Characteristics and Operating Conditions of Aerobic MBR Process (Submerged Membrane)
Synthetic Domestic Industrial Synthetic Synthetic Industrial MF Hollow fiber Polyethylene 0.1 0.3 2080 4.5 18 MF Hollow fiber Polyethylene 0.1 0.6 40 25 2.5 12.5 MF Hollow fiber Polyethylene 0.1 0.6 80 5 4 8.33 MF Hollow fiber Polyethylene 0.1 0.27 27 2530 10.918.2 6.73.5 MF Hollow fiber Polyethylene 0.10.2 410 8 16.6 8.3 5.5 MF Hollow fiber Polyethylene 0.1 0.9 40 MF Hollow fiber Polyethylene 0.1 0.3 13 1622 716 6 23-24 1011 9 Domestic MF Hollow fiber Polyethylene 0.2 1 20/44/96 29-31 1214 6/14/27

Wastewater type

Membrane configuration

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Yamamoto et al., 1989 Takeuchi et al., 1990 Yamamoto et al., 1991 Chiemchaisri, Chiemchaisri et al., 1992, 1993 et al., 1992, 1993 Benitez et al., et al., 1995

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Membrane material Pore size (m) Filtration area (m2) Transmembrane pressure (kPa) Temperature (C) MLSSa (kg/m3) Flux (l/m2.h) Frequency of cleaning Reference

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Parameshwaran et al., 1998

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TABLE 6 Characteristics and Operating Conditions of Anaerobic MBR Process


Pulp Brewery Wheat starch Synthetic Industrial MF UF MF UF (P and F) UF (tubular) MF (hollow fiber/tubular) MF (P and F) 2 106 12 Polysulfone 3 106 0.02 0.8 49 and paper High strength SS Distillery

Wastewater type

High strength UF UF

Membrane MF plate and frame Organic UF (tubular) Polyethersulfone 40,000 0.44 1.5 160 50 40 3540 30 28 FakhrulRazi, 1991 1991 1994 16.25 25s/67 min. Kimura, 12.5 1/23 weeks Kimura, Strohwald and Ross, 1992 3138 37 16.9 35 15 37.5113.3 0.45 0.012 2 150 15.8 30 Anderson, 1984 Nagano et al., 1992 10,000 0.1 54 0.9 2 1 06 20 1.0 PVDF 0.1 1.52 100 35 15b Harada et al., 1994 37 3545

configuration

2 106 7.6 Seyfrid and Broockmann, 1995 Miami et al., 1991

20,000 0.22 Kitamura, 1994

10,000 Hall et al., 1995

Membrane material Pore size (Dalton/m) Filtration area (m2) Cross flow velocity (m/s) Transmembrane

pressure (kPa) Temperature (C)

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MLSSa (kg/m3) Flux (l/m2.h)

Frequency of cleaning Reference

Mixed-liquor suspended solids. Mixed-liquor volatile suspended solids, MLVSS.

adhesion, thus the flux rate is higher. Long lifetime, ability to withstand rigorous chemical cleaning, and high operating pressures are some of the advantages of ceramic membranes. The comparisons provided in Tables 4 to 6 indicate that membrane flux depends not only on the selection of membrane (type, geometry, etc.), but also on operating conditions such as transmembrane pressure (TMP), crossflow velocity, etc. Therefore, membrane selection (investment and replacement cost) and operating conditions (energy, cleaning requirements, etc.) dictate the cost of filtration.

1. Transmembrane Pressure
Membrane filtration performance is affected by the resistance of the membrane itself and the resistance created by the fluid under going filtration. The resistance model is illustrated in Figure 4. Based on this model, the permeation flux is determined by flow resistance in series as in Equation 1.

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J=

P Rt

(1)

where J, permeate flux (m3/m2.s); P, transmembrane pressure (Pa); , viscosity of the permeate (Pa.s); Rt, total resistance for filtration (l/m).

FIGURE 4. Resistance in series model. Rm, membrane resistance; Ref, external fouling resistance; Rp, polarization layer resistance; Rif, internal fouling resistance.

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As depicted in Figure 4, total resistance is a function of the intrinsic membrane resistance (Rm), the polarization layer resistance caused by the concentration gradient (Rp), external fouling resistance formed by deposited cake layer from physicochemical interactions of solids with the membrane (Ref), and internal resistance due to materials absorbed into the pores (Rif). Equation 1 becomes:

J=

Rm + RP + Ref + Rif

(2)

Because it is difficult to clearly discriminate between Rp and Ref, these two terms are combined into a single term, external resistance (Re). Thus
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J=

Rm + Re + Rif

(3)

Pressure applied for filtration influences cake compressibility and thus the resistance caused by the cake layer Re. Therefore, Re can be written as a function of transmembrane pressure (Re = P). Where is a function of the cake layers mass transfer properties. Equation 3 becomes:

J=

Rm + Rif + P

(4)

For a given fluid, the permeate flux is a function of transmembrane pressure, and Equation 4 shows two distinct pressure-dependent (at low pressure) and pressure-independent (at increased pressure) regimes. In the pressure dependent part, permeate flux is more or less proportional to applied pressure. In the pressureindependent zone, permeate flux is mainly dictated by cake layer resistance (Figure 5). In continuous operation, permeate flux at low transmembrane pressure is higher than that at higher transmembrane pressure. This seems to indicate that the specific resistance of the solids boundary layer is a strong function of the applied suction pressure, and an increase in resistance to filtration more than offsets increased driving force (Bentez et al., 1995; Parameshwaran et al., 1998). This emphasizes that filtration should be carried out at a low transmembrane pressure.

B. Crossflow Velocity As shown in Figure 5, increasing the transmembrane pressure above the pressure-independent part is useless because the flux does not increase any further.

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FIGURE 5. Schematic representation of flux vs. transmembrane pressure.

However, in this region flux is mainly dictated by the cake layer formation and any force that disturbs it can influence the flux rate. By increasing the crossflow velocity (in external circuit membranes) or agitation around the membranes (in submerged membranes), the cake layer-forming materials can be swept away. A linear relationship between the flux and the crossflow velocity at constant TMP for the filtration of biomass of an anaerobic digester treating brewery effluent has been reported (Strohwald and Ross, 1992). With increased crossflow velocity, an improvement in flux and shift in the pressure-independent zone (Figure 6) was also reported (Magara and Itoh, 1991). However, a study by Ghyoot and Verstruete (1998) with anaerobically digested sludge indicated that an increase in crossflow velocity had only a minor affect on the permeate flux. Shear caused by high crossflow velocity may lead to floc rupture and higher dispersion of biomass. Therefore, enhanced organic and oxygen mass transfer within the biomass can help increase process efficiency. Improved efficiency of an anaerobic digester was reported by Pillay et al. (1994). In this study, the solid concentration in the digester was increased from 2.6 to 5.5%, and the HRT decreased from 26 to 14 h, while the SRT was maintained at 26 days. Observations reported by other researchers contradict this observation (Ghyoot and Verstruete, 1998; Brockman and Seyfried, 1993). According to these investigations, the excess mechanical stress caused during crossflow damaged the interaction between different species in the anaerobic consortia, particularly the symbiosis in the acidogenic and methanogenic stages. However, these authors agree that the use of a centrifugal pump for crossflow would have destroyed the sludge structure faster than any other kind of pump. It can be concluded from these observations that although

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FIGURE 6. Relationship between permeate flux and driving pressure at various velocities.

crossflow can help improve process performance, equipment selection is an important factor in alleviating any negative impact on the process.

C. Effects of Aeration on Flux Although aeration basically serves the purpose of providing the air required for biodegradation and keeping the biomass dispersed throughout the reactor, it serves another important role in submerged MBRs. Turbulence induced by aeration creates crossflow velocity in the vicinity of the membrane module. Therefore, it can be anticipated that by augmenting the air flow rate or increasing aeration intensity (airflow rate per unit area) by concentrating the membrane modules over a smaller floor area, cake removal efficiency can be improved and with it the flux. However, Udeda et al. (1997) found that although an increase in the air flow rate partially stimulated cake removal efficiency, there was a critical value beyond which an increase in air flow rate had virtually no effect.

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D. Membrane Fouling In all practical membrane filtration applications, as the resistance increases the flux will decline. This increase in resistance may be due to changes in Rm, Rif, Re or all three (Equation 4). If the flux decline is not reversible by simply altering operating conditions, it is termed fouling (Fane et al., 1989). This is a major problem in membrane filtration because it reduces productivity, shortens membrane life (often due to the need for aggressive cleaning agents), and impairs the fractionation capability of the membrane. Membrane fouling can result from the precipitation of less soluble inorganic species (scaling), adsorption of organic substances (organic fouling), and adhesion and growth of microbial cells at the membrane surface (bio fouling). Studies with anaerobic sludge filtration show almost no cake layer observed on the surface of the inorganic membrane, but inorganic fouling inside the pores (Rif = 0.9 Rt) plays a key role in limiting flux (Kang et al., 1996). For organic membranes, a 13-m cake layer formed due to its much rougher surface structure. Howver, the amount of inorganic foulant deposited was one-fourth that observed in a ceramic membrane (Kang et al., 1996). Because MBRs use organic membranes, biofouling is a major concern. Biofouling includes (Winfield, 1979): The adsorption of macro molecules, which lead to a conditioning film on the membrane (humic substances, lipopolysaccharides, and other products of microbial turnover) Primary adhesion by fast-adhering cells from the micro flora of the mixed liquor colonization and growth of bacteria with subsequent adhesion of a number of different species, exertion of extracellular polymers (slime), and the development of a biofilm. The application of continuous high filtration force (TMP) may protect the cake layer against hydraulic forces. To understand the early phase of biofouling, consider a system of three components: microorganism (species, composition of mixed population, hydrophobicity, surface charge, etc.), membrane surface (chemical composition, surface charge, hydrophobicity, roughness, porosity, pore size, etc.), and mixed liquor (suspended matter and colloids, viscosity, pressure, shear forces, boundary layer, flux rate, etc.). Typical methods used to reduce fouling effects include control over operating conditions (low pressure, high turbulence, and intermittent filtration), backwash (with permeate or air or both), and chemical cleaning. However, when fouling becomes too extensive and membrane productivity is lowered beyond compromise, the membrane must be replaced. Biomass filtration with an evenly distributed pore on an isoporous and highly porous, hydrophilic smooth membrane surface operated at low to modest pressure

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can reduce fouling (Fane et al., 1989). It has also been suggested that the membrane should be negatively charged or neutral to limit biomass adsorption (Shimuzu et al., 1989).

E. Mode of Operation Flux decline can be reduced by various means of operating control. Instead of continuously filtering, intermittent filtration can reduce the compression of the cake layer, thus resistance is reduced and better flux maintained (Yamamoto et al., 1989; Cheiemchaisri et al., 1992). In certain cases, permeate backwashing has also been advocated (Trouve et al., 1994 a). Extensive studies on intermittent operation with air backwashing indicate improved flux rate compared with continuous operation (Visvanathan et al., 1997; Parameshwaran, 1997). The results of intermittent filtration with air backwashing are shown in Figure 7.

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F. Module Arrangement Module arrangement influences turbulence at the membrane surface. Due to their high packing density, hollow fiber membranes are most likely to be used in submerged membrane bioreactors. In hollow fiber membranes, the main reason for

FIGURE 7. Comparison of net cumulative permeate volume (after 8 h) in different modes of operation (15* = 15 min without air diffusion).

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flux decline is the accumulation of particles in the spaces between fibers. Solid accumulation under different packing density of fibers indicates that there are four conditions: (1) totally dispersed, (2) partially accumulated, (3) completely accumulated, and (4) surface clogging. Particle accumulation between fiber spaces can be avoided if a packing density lower than a critical value is used (Kiat et al., 1992).

G. Viscosity Viscosity of permeate and mixed liquor affects permeation flux. An increase in permeate viscosity directly affects the filtration flux, as shown in Equation 4. Because the permeate is essentially water, flux is mainly affected by operating temperature. However, sludge viscosity also indirectly influences flux (Praderie, 1996). The degree of turbulence (indexed by the Reynolds number) in the vicinity of the membrane surface and the velocity gradient along the membrane surface during crossflow can be affected by sludge viscosity, which is in turn affected by concentration. Krauth and Staab (1994) suggest an exponential dependence between sludge concentration and viscosity for aerobic sludge. Similar results for anaerobic sludge have also been reported (Ross et al., 1990). Magara and Itoh (1991) found that a semilogarithmic relationship can be used to describe the influence of biomass concentration on the limiting flux.

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J = 1.571 log(MLSS) + 7.84

(5)

where J, permeate flux (m/d); MLSS mixed liquor suspended solid concentration (mg/l). The relationship in Equation 5 was developed for a concentration ranging between 5 and 15 g/l. In contrast is an observation by Ross et al. (1990) on anaerobic sludge filtered with ultrafiltration. They found that flux was relatively stable up to a concentration of 40 g/l, but then decreased sharply and stabilized at about 60 g/l.

V. APPLICATION OF MEMBRANE SEPARATION BIOREACTORS IN AEROBIC WASTEWATER TREATMENT The activated sludge process was invented in 1914 by Edward Arden and William Lockett of Manchester Corporation in England (Arden and Lockett, 1914) and is now the most commonly used biological wastewater treatment system. Capture of biological solids is essential to achieve low-effluent BOD and to control the accumulation of biomass. Significant improvements in solids separation have had a noticeable impact on the efficiency and reliability of biological processes. For nearly 4 decades researchers have studied various aspects of membrane-

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coupled bioreactors. Yamamoto et al. (1989) were the first to introduce submerged membranes in an aeration tank for solid/liquid separation. Prior to this, researchers concentrated on crossflow membrane filtration in external circuits. These early studies (e.g., Smith et al., 1969) used ultrafiltration membranes in the external membrane circuit type and, although there are still studies with ultrafilters (e.g., Muller et al., 1995; Chaize and Huyard, 1991), the present trend is toward microfiltration.

A. Bioreactors with Membrane in External Circuit A pilot plant with a completely mixed biological reactor (4.5 l) connected to an ultrafiltration module was used by Chaize and Huyard (1991) to treat domestic wastewater. Air was supplied to the reactor at a rate of 80 l/h and the mixer operated at 800 to 1200 rpm. The ultrafiltration membrane module (molecular weight cut off 50,000 D) was operated with a cross-flow velocity of 1.5 m/s and 1 to 2 bar transmembrane pressure. Concentrate from the membrane module was returned to the reactor. Experiments were carried out in two runs. The first run was carried out for 160 days with an HRT of 8 h and an SRT of 100 days. After 25 days of operation, biomass concentration reached a steady state with MLSS concentration varying between 8000 and 10,000 mg/l. The effluent COD was reported to be less than 30 mg/l, while the influent COD was in the range of 250 to 550 mg/l. The effluent TKN was less then 10 mg/l, while the influent TKN was in the range of 65 to 150 mg/l. This nitrification phenomenon was observed 14 days after start up. The F/M ratio varied between 0.06 and 0.1 kg COD/kg MLSS.d. For the second run, the HRT was varied 8, 4, and 2 h, with corresponding SRTs of 100, 100, and 50 days in order to study the steady state of biomass concentration under different operating conditions. Over 200 days of operation, the biomass concentration increased slowly up to 30 days after which membrane permeability decreased. Changes in operating conditions (HRT and SRT) had no effect on carbonaceous removal. However, at the start of the operation, TOC accumulated in the bioreactor. As the biomass concentration increased, the TOC decreased; however, accumulation of TOC again increased when HRT was reduced. This could be due to the accumulation of either bacterial products or raw water components. Under different operating conditions, this phenomenon was observed by several other researchers (refer to Table 7). Although changes in operating conditions disturbed the removal of nitrogen compounds, after a period of adaptation the removal was maximum for each HRT studied. Studies by other researchers on the operating conditions and performance results for membrane coupled bioreactors with the membrane in an external circuit are presented in Table 7.

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B. Bioreactors with Submerged Membranes A series of laboratory scale experiments were carried out by Yamamoto et al. (1989) to determine the feasibility of direct membrane separation in an activated sludge aeration tank. The study was carried out with a 0.1-m-pore-size hollow fiber membrane. Short-term experiments with constant MLSS concentration revealed high suction pressure (80 kPa) led to rapid reduction in flux. During longterm experiments, continuous suction caused severe clogging of the membrane module with an increasing pressure difference up to 100 kPa. A stable flux was observed for 120 days at a volumetric loading of 1.5 kg COD/m3.d using intermittent suction at a low pressure of 13 kPa. COD removal of more than 90% was reported despite the intermittent aeration. However, nitrate removal varied considerably above 80% and the denitrification efficiency ranged from 20 to 60%. Intermittent aeration did not change the denitrification efficiency, indicating that the dissolved oxygen could not be depleted in such a short nonaeration time. From the analysis of the reactor supernatant and effluent, it was found that the membrane acts as a separator removing a certain amount of dissolved and colloidal COD. During steady state operation, the F/M ratio was 0.1 kg COD/kg MLSS.d and the critical organic loading was estimated at 3 to 4 kg COD/m3.d to maintain both stable flux and an aerobic condition. Absence of a recirculation pump led to a very low power consumption of 0.007 kWh/m3. Chiemchaisri (1990) investigated an activated sludge process with a 0.1-m hollow fiber membrane module for solid-liquid separation to treat low-strength domestic wastewater. A comparison was made of the performance of the membrane bioreactor under different operating conditions, such as nonaerated and aerated, with different initial hydraulic retention times of 1, 3, and 6 h (with corresponding permeate flux of 4.17, 1.38, and 0.7 L/m2.h). The process was operated at intermittent extraction, 10:10 min operating time. The magnetic stirrer was employed in nonaerated condition to keep MLSS in suspension. The nonaerated bioreactor had an advantage over the aerated condition at initial HRTs of 3 and 6 h, because lower energy was required to give similar effluent quality and process stability. However, at an HRT of 1 h (or higher permeate flux, 4.17 L/m2.h) aeration was required to prevent membrane clogging. Flux of 4.17 L/m2.h seems to be a critical value between severe clogging and nonclogging conditions. At lower flux, no clogging was observed under nonaerated and aerated conditions. The quality of the permeate in terms of COD was independent of the low volumetric organic loading in the range of 0.2 to 2 kg COD/m3.d. Because of the long solid retention time (SRT), the process was stable and steady, and COD removal efficiency was similar in all experimental conditions. Performance of the 0.03-m pore size with 9 m2 surface area of hollow fiber membrane was also investigated in a pilot-scale unit (Chiemchaisri et al., 1993) Two hollow fiber membrane modules were immersed in an aeration tank that was fed diurnally with domestic wastewater. A suction pump was used at 10:10 min intermittent operation to extract the permeate through the membrane. The effect of
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a jet aeration period (0.5 and 1 h) and a jet aeration pattern (15 min two times a day and 30 min once a day) was investigated. The jet aeration flow rate was 20 l/ min. The settling of solids to the bottom of the bioreactor and the creation of anaerobic conditions resulted in the division of the bioreactor into two zones, aerobic and anaerobic. This resulted in low MLSS in the aerobic zone that could have reduced membrane clogging. The mean hydraulic retention time (HRT)was determined after the permeate flux reached a steady state. The average flux was around 4.17 l/m2.h, corresponding to an average HRT of 1 day under diurnally varied loading. The diurnal variation had a minor effect on the nitrification process because more than 80% nitrification was observed throughout the experiment. The MLSS in the bioreactor was affected by the air flow rate. Optimum air flow rate in this experiment was taken as 7.5 l/min, which provided sufficient oxygen for the microorganisms and maintained low MLSS in the aerobic zone. Direct membrane separation using hollow fiber membranes in an activated sludge process was investigated on a pilot scale by Chiemchaisri et al. (1992). The experimental set up used for this study is shown in Figure 8. The system consists of two parts, the main bioreactor and a separation unit. A separation unit of 10 l volume was immersed in the main bioreactor, which had a 62-l volume. Two hollow fiber membrane modules 0.03 and 0.1 m pore size) of 0.3 m2 surface area each were placed in the separation unit. Paddles driven by a motor provided a cross-flow of mixed liquor across the membrane surface at a speed of 290 rpm in 10-s cycles in alternate directions. By providing highly turbulent conditions within the separation zone in conjunction with jet aeration inside the membrane module, sludge accumulation on the membrane surface and inside the module was reduced. The permeate flux obtained after 330 days of operation was 8.33 l/m2.h (0.2 m3/ m2d) under intermittent suction. A high degree of organic matter reduction (> 85%) was observed with 20.8 and 16.5 mg/l of COD in the effluent during continuous and intermittent aeration modes, respectively. The degree of nitrification and denitrification was above 90% during intermittent aeration (90 min aeration and 90 min rest) at a dissolved oxygen level of 4 to 5 mg/l. However, at similar intervals of intermittent aeration at a low dissolved oxygen level (1.5 to 2 mg/l), a reduction in nitrification and denitrification efficiency (80%) resulted in 4.9 mg/l of total nitrogen in the effluent. In addition, a virus reduction of 4 to 6 log number was reported. Buissson et al. (1998) reported on the concept of immersed membranes for upgrading wastewater treatment plants. The pilot plant consisted of two reactors in series, the first one under anoxic conditions and the second one with aeration. In this denitrification-nitrification mode, the unit was fed with municipal wastewater. The hollow fiber modules were directly immersed in this aerated tank. Aerators were positioned at the bottom of the membrane modules to provide the required amount of air to promote turbulence and increase mass transfer in the vicinity of the membranes. The membranes were backwashed with treated water at regular intervals with permeate to remove the filter cake. The researchers reported a sludge
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FIGURE 8. Schematic of experimental system. (From Chiemchaisri, 1990.)

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concentration of 15 g MLSS/l and a volumetric loading of 1.2 kg COD/m3/d with 96% COD and 95% total Kjeldahl nitrogen (TKN) removal. In parallel with the development of hollow fiber submerged membrane bioreactor systems, Japanese researchers developed Kuboto submerged flat plate membrane systems. This process has been tested on a pilot scale in the U.K. (Churchouse, 1998; McCann, 1998). In this system (shown in Figure 9), flat plate microfiltration membrane panels housed within a rectangular box are submerged in an activated sludge tank and a coarse bubble aeration system is placed at the bottom of the membrane module. The aerated sludge that rises between the panels provides sufficient recirculation of sludge at the membrane surface. It also generates an upward cross-flow over the membrane surface and keeps surface fouling to a minimum. The permeate from the system is obtained either by a low-pressure (0.1 bar) suction pump or by gravity. The module arrangement and the aeration system require very little membrane cleaning. Using a mechanical water jet, the modules are washed once a year. In addition, this system needs in situ cleaning two to four times per year for flux improvement. The system was tested in degritted sewage with a denitrification and nitrification arrangement with wide variation in effluent quality (30 to 2100 mg/l BOD and 100 to 4000 mg/l COD) (Churchouse, 1998). The final effluent from this process consistently met a 5:1:1 (BOD:SS: NH3N) standard with 96% removal achieved of COD and BOD. The average sludge production was 0.3 kg/kg BOD, which is approximately 40% of the normal activated sludge process production rate. A comparison of operating conditions and corresponding performances of several submerged membrane bioreactors is presented in Table 8.

FIGURE 9. Schematic of the Kubota membrane unit operation and panel construction.

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C. Membrane as Air Diffuser and Clarifier An alternative method to improve performance of membrane bioreactor systems uses the membrane in alternate cycles to filter and aerate with both external circuit and submerged membranes in the bioreactor. Scott and Smith (1997) studied the alternate functioning of aeration and separation with a microfiltration ceramic membrane (0.2 m) in an external circuit of a membrane coupled bioreactor for remediating food process industry wastewater (Figure 10). It was concluded that a 0.2-m membrane provided markedly superior fine bubble aeration to traditional aerators and kept permeate suspended solids below 50 mg/l, despite an input of 1500 to 3800 mg/l. At 25C, influent COD loading of 13,330 mg/l and BOD of 6500 mg/l, removal efficiencies in excess of 95% were obtained. In addition, ammonia nitrogen was reduced from 9 to 10.2 mg/l to < 0.3 mg/l and total phosphorous from 20 to 21.2 mg/l to < 4 mg/l. This study suggested the need to determine optimum air supply rate and bioreactor HRT. Furthermore, although successful runs were conducted without nutrient addition, nutrient limitation appears likely in most industrial wastes. Nutrient

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FIGURE 10. Schematic of ceramic membrane-based bioreactor.

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addition therefore may provide further enhancement of degradation rates, although any improvement would have to be offset against the costs of additives. Visvanathan et al. (1997) used a 0.1 m hollow fiber membrane module directly in the reactor for solid-liquid separation of domestic wastewater with permeate flow outside-to-inside arrangement. During short-term experiments, the effect of transmembrane pressures, intermittent mode of operation and duration of air diffusion were investigated to determine the optimum conditions corresponding to a high and constant flux obtained. Variations in transmembrane pressure were studied with values of 13.3, 21.3, 32.0, and 41.0 kPa. It was found that a transmembrane pressure of 13 kPa was the limiting pressure for all experiments. The different operating modes studied by varying duration of effluent filtration and air diffusion through the membrane were 5:5, 10:10, 15:15, 30:30, 60:60, and 15:15* (15* = 15 min without air). The results show that an operational mode of 15:15 min provides the best results. Although cyclic operation with air diffusion could not completely eliminate clogging, the air diffusion through the membrane backwash technique in this mode of experiment could improve the flux by up to 370% compared with a continuous operation. These experimental results also indicated that the transmembrane pressure increased according to cake formation on the membrane. Steep increases in transmembrane pressure were observed even under air diffusion conditions. Periodic chemical cleaning was needed in order to recover the permeate flux, which exhibited good quality in terms of very low SS and BOD. During the experimental runs the sludge was not removed from the reactor, and more than 90% reduction in COD with influent concentration of 200 to 300 mg/l and effluent concentration below 20 mg/l was achieved in all runs. The TKN removal was more than 90%, and total phosphate removal was approximately 50% in all runs. The MLVSS/MLSS ratio in the bioreactor was in the order of 20 to 30%. Solid matter mass balance calculation indicated a steady accumulation of inorganic components within the reactor. The lower fraction of active microorganisms in the bioreactor did not show any significant effect on the process efficiency. Nevertheless, it is anticipated that in longer runs it might, and periodic sludge draining therefore would be advisable. The possibility of using microfiltration hollow fiber membrane modules as air diffusers and solid/liquid separators in alternating cycles for activated sludge process treating domestic wastewater was reported by Parameshwaran et al. (1998). The activated sludge system consisted of an anoxic and oxic zone for better nitrogen removal. Two hollow fiber microfiltration modules with a pore size of 0.2 m were immersed in an 80-l oxic tank (MBR) to effect the direct solid/liquid separation (Figure 11). Filtration and high-pressure air backwashing were employed in alternating cycles to improve the flux rate. Backwashing the membrane with air was used to aerate the activated sludge in the reactor. This achieved distinct advantages of membrane declogging and aerating reactor contents simultaneously.
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FIGURE 11. Membrane as air diffuser and solid/liquid separator.

In short-term experimental runs, it was found that membrane module are better air diffusers than stone air diffusers. It was also found that increased backwash air pressure leads to improved flux rate. The efficiency of membrane coupled bioreactor systems at different hydraulic retention times of 15, 10, 6, and 3 h was studied in long-term experiments. Wastewater was fed to the anoxic tank that passed into the MBR. The contents of the MBR were recycled to the anoxic tank to effect denitrification. The average MLSS concentration in the system varied between 12,000 to 14,000 mg/l, and the sludge age in the MBR was maintained at 50 days throughout the study. The desired HRT could be maintained at 15, 10, and 6 h with a moderate transmembrane pressure (< 42 kPa), but not at 3 h. Irrespective of the operating conditions, in all experiments COD, BOD, TKN and total nitrogen removal of more than 95, 98, 95, and 80%, respectively, was achieved. This study established that using a hollow fiber membrane capable of air backwashing to solid/liquid separation leads to aeration of mixed liquor and declogging of membrane modules simultaneously and that conventional aerators could be eliminated. By using anoxic/oxic systems, efficient total nitrogen removal can also be achieved. VI. APPLICATION OF MEMBRANE BIOREACTORS IN ANAEROBIC WASTEWATER TREATMENT Since its introduction more than 4 decades ago, anaerobic treatment has become a well-established process for concentrated industrial wastewater and
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municipal sludge management. In recent years, there has been a better understanding of the microbiology of this process and improved reactor design has made it possible to consider them for treatment of dilute low-strength wastewater. The major difficulty in anaerobic wastewater treatment processes is the retention of a sufficient quantity of an active biomass due to their slow net growth rates. As a result, anaerobic systems require a longer minimum solids retention time (SRT). Operating below this minimum SRT would result in microorganisms being washed out of the system at a faster rate than the growth rate leading to system failure. Anaerobic treatment is not popular due to its low efficiency and inability to meet discharge regulations despite the advantages of generating methane fuel gas and low sludge yield. Also, these systems are unable to cope with shock loading and wide fluctuations in influent flow. The loading rates in anaerobic wastewater treatment systems are mostly dictated by the biomass retention in the reactor. High biomass retention will give good reactor performance, leading to better gas yields and better-quality effluent. A lower retention capability will lead to a longer hydraulic retention time (HRT), thus requiring reactors of larger volume and higher cost. These problems could be overcome if the biomass in the reactor can be retained longer than the minimum SRT, thus increasing biomass concentration. For dispersed growth anaerobic systems, a high concentration of biomass retention was achieved through improved separator performance by the use of chemical coagulants and modifications in processes and component design. Apart from this, various anaerobic reactor configurations, such as anaerobic filters, fluidized bed reactors, upflow anaerobic sludge blanket reactors (UASB), rotating contactors, etc. are advocated with a view to longer sludge retention times and shorter hydraulic retention times. Although all these systems needed less space compared with the suspended growth anaerobic systems. Except UASB all other systems use part of their space to accommodate the media on which biomass attached. However, the problems associated with UASBs are related to the requirement for a suitable seed sludge that can be granulized and maintenance of an appropriate organic loading rate and close control of environmental conditions. In this situation, the application of membrane separation for anaerobic wastewater has some distinct advantages: Increasing the biomass concentration without increasing the reactor volume irrespective of the granulation of sludge Colloidal/suspended solid-free, good-quality effluent. A number of membrane anaerobic systems were tested mostly with industrial wastewater to determine their performance Improved treatment efficiency that can easily meet standards since colloidal matters and macromolecules are retained in the bioreactors by the membranes and completely degraded Intermediate toxin removal at a faster rate to prevent system failure, because all the microorganisms, including slow-growing methonogens, are retained
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Some studies have indicated that a higher methane production rate was obtained in anaerobic MBR

A. Treatment of Domestic Wastewater in Membrane Coupled Anaerobic Process Grethlein (1978) demonstrated how a septic tank-membrane system is feasible for the treatment of domestic wastewater. The experimental set up used in this study is shown in Figure 12. A two-compartment rectangular tank with a total volume of 106 l was constructed, and a minimum flow rate of 2.65 l/min was applied. Operating pressure was in the range of 345 to 1030 kPa (50 to 150 psi). By using the surge capacity of the septic tank, the average volumetric flow rate of the inlet and outlet were matched. Two types of membrane module were used (a flat sheet membrane module and a helicore reverse osmosis unit). In order to control concentration polarization at the membrane surface and to mix the contents of the septic tank, the circulation flow (cross-flow) over the membrane surface was kept much higher than the permeate rate. It appears that with a 2:2 operating cycle (2 min ON, 2 min OFF), it was possible to maintain a steady flux of about 20.42 l/m2h with a cross-flow velocity as low as 22.9 cm/s. During the off period of the cycle (during the off period, feed side pressure is released by opening the bypass valve) when backflow occurred, some noticeable solids were floated off, but not enough to clean the entire membrane surface. The spontaneous break-up of the gel layer, which results in cleaning

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FIGURE 12. Experimental setup for septic tank effluent treatment.

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the surface of the membrane, is a self-cleaning method unique to the cyclic operation procedure, and in the long run is probably the most important mechanism for achieving long-term practical flux levels. The water quality of the treated effluent is similar, if not better, than that of secondary treatment effluent. For example, E.coli and turbidity are below the detection limit, while BOD is reduced by 85 to 95% for an influent concentration of 270 mg/l. A particular feature of this system is its ability to reduce the initial feed nitrate concentration of 3.5 mg/l by about 75%. The anaerobic rate of digestion of organic carbon in the septic tank is enhanced by a factor of 3 to 4 because of the increased concentration of microorganisms and substrate caused by membrane. The pH stability of the digester is excellent (6.5 to 7.2), even with intermittent loading. The sludge accumulation was less than in an ordinary septic tank.
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B. Treatment of Industrial Wastewater in Membrane Coupled Anaerobic Process A comprehensive study using ADUF( (anaerobic digestion-ultrafiltration) processes for the treatment of different industrial wastewater was carried out in South Africa (Ross and Strohwald, 1994). In this process, a 9-mm tubular polyethersulfone membrane at a pressure of 500 kPa was used. The ADUF process consists of two main unit operations: an anaerobic digester coupled with an external pressure driven ultrafiltration unit. Some of the studies carried out with this unit are described below.

1. Wine Distillery Wastewater


A pilot-scale anaerobic digester with an external ultrafiltration membrane to treat wine distillery wastewater (37,000 mg COD/l) was reported by Ross et al. (1990). A pilot plant with a digester and external UF unit is shown in Figure 13. The 2.4 m3 digester operated at a MLSS concentration of 30,000 mg/l, and prior to the installation of the UF module could only be fed with wine distillery waste at a volumetric loading rate of some 4 kg COD/m3.d at 35C. A UF module with a total membrane area of 1.75 m2 was used for the test at an inlet pressure of 400 kPa. The high rate of sludge recirculation through the UF unit to comply with a cross-flow velocity of 2 m/s resulted in a permeate volume (2.4 m3/d) well in excess of that of the substrate feed rate (0.3 m3/d) to the digester. The oversized UF unit was accommodated by wasting a volume of permeate equivalent to the daily feed volume, and by recycling the excess permeate back to the digester. All the sludge concentrate was returned to the digester. The experimental results obtained on the ADUF system include the following:

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An extremely high initial permeation flux of 62.5 l/m2.h at 400 kPa inlet pressure that gradually decreased to 37.5 l/m2.h after 7 months continuous operation. Temporary substitution of the original module by a new one also gave a flux of 37.5 l/m2.h, indicating that the flux decline was not caused by membrane fouling, but by changes in the digester contents, for example, the SS in the digester increased over the 7 months to 50 kg/m3 from an initial concentration of 30 kg/m3 Building up of biomass occurred in the digester, with a concomitant increase in the permissible volumetric loading rate notwithstanding the poor settleability of the sludge. During the study period, the load rate increased from 4 to 12 kg COD/m3.d The operating flux was successfully maintained for a period of several weeks before membrane cleaning was necessary The degree of COD removal was 93%, based on a feed and effluent concentration of 37.0 and 2.6 kg/m3, respectively. Table 9 presents the information on principle operating conditions and results of various reported pilot- and full-scale ADUF plants. Other studies have looked at the possibility of using membrane coupled anaerobic digesters for industrial wastewater treatment. Ultrafiltration membrane separation for anaerobic industrial wastewater treatment was studied by FakhrulRazi (1994). The study was conducted at a temperature of about 35C, a pressure range of 100 to 300 kPa and with minimal pH control (the pH ranges from 6.8 to 7.4 throughout the study). The reactor was subject to different organic loading rates

FIGURE 13.

Diagram of pilot-scale ADUF process applied for anaerobic treatment.

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TABLE 9 Mean Operating Criteria of ADUF Plants Treating Various Industrial Effluents

Parameters Unit Brewery Malting

Wine distillery Egg process

Maize process

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37
From Ross and Strohwald, 1994.

Volume of digester Operational period Feed COD Permeate COD COD removal Space load rates Sludge load rate HRT Temperature MLSS Membrane area Flux Inlet pressure Crossflow velocity Tube diameter 0.05 3 6.7 0.18 97 17.0 0.7 0.8 35 3050 0.44 1040 340 1.5 9.0 2.4 18 37 0.26 93 12.0 0.58 3.3 35 50 1.75 4080 400 2.0 12.7 3.0 5 3.5 0.8 77 5.0 0.5 0.8 35 10 9.6 2040 500 1.8 9.0 80 8 8 0.35 95 6.0 0.33 1.3 30 1030 200 1530 500 1.8 12.7

m3 month kg/l kg/l % kg COD / m3.d kg COD/kg VSS.d day C kg/m3 m2 L/m2.h kPa m/s mm

2610 36 415 0.3 97 3.0 0.24 5.2 35 23 800 1070 600 1.6 9.0

(OLR) ranging from 12 to 20 kg COD/m3.d. The SRT was achieved by deliberately wasting reactor sludge from the system. The SRT range was between 83 to 53 days. Six steady states were attained over a MLSS range of about 31,000 to 38,000 mg/l. It was found that rate of gas production in the reactor increased with increasing OLR. The methane content of the reactor gas declined from 65.3 to 57.1%. Methane yield ranged from 0.26 to 0. 29 m3 CH4/kg COD. However, no sudden increase in volatile acids concentration were recorded during the study, indicating that the anaerobic system coped quite well with the increasing loading rates. The reduced methane content could be due to the much higher influent COD, resulting in a higher rate of carbon dioxide formation by the acid-forming bacteria in the reactor. The treatment efficiency of the membrane anaerobic system showed a consistent COD removal of above 96%. The highest influent COD applied to the system was 84,010 mg/l, and the corresponding effluent COD for this was 3100 mg/l, which represents a COD removal of 96.3%. It was further observed that MLSS and MLVSS increased with increasing OLR. The rise in MLVSS concentration indicates that the bacterial population, including methanogenic bacteria, increased with the higher influent COD applied. Further increases in the OLR were possible in order to achieve further bacterial growth leading to a much higher MLVSS concentration in the reactor. During the experimental study, the SRT was reduced from 83.3 to 58.8 days due to the increase in the deliberate sludge wastage rate from the reactor. This was necessary in order to offset the drop in membrane flux from the UF module over the period of the study. The results indicate that a membrane anaerobic treatment system is suitable when higher biomass retention and its treatment efficiency is expected. The study showed that the incorporation of membranes in a system enable it to retain active bacterial populations and produce a clear effluent as final permeate. The system also showed that it was capable of higher loading rates and has yet to achieve its maximum treatment capability. This was a result of good control of bacterial populations in the reactor provided by the UF membranes. Throughout the study there was negligible biomass loss through the effluent/permeate. In an experiment by Harada et al. (1994), the permeate flux decreased significantly as the cultivation time elapsed. This may have been brought about by the formation of a gel layer on the membrane surface. This phenomenon was caused by insolubilization of high molecular organic substances. In addition, the increase in MLSS enhanced the deposition of cells to the gel layer matrix and accelerated the deterioration of the flux. Although washing with water eliminated some of the gel layer, the permeate flux was not restored to 100% of the initial level after each wash. In the membrane bioreactor the major portion of the organics present were substances with molecular weights (MW) as large as 106, while the permeate consisted of substances with MWs less than 1500. This large difference in molecular size between the concentrate and the permeate implies that the membrane was

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capable of not only separating suspended or colloidal matters but also fractionating soluble organics by molecular size. The exclusion of higher molecular size materials from the permeate is attributable to the formation of gel layers on the membrane surface. The formation of a gel layer is responsible for the decline in permeate flux, although it is useful for production of high-quality effluent. A comparison of different studies with anaerobic bioreactors followed by membrane separation is presented in Table 10.

VII. ECONOMICS OF THE MBR PROCESS The success of any process is ultimately determined by its economic benefits and higher investment and operating costs, which hinder the progress of MBR processes. However, cost of potable water and the disposal cost of wastewater resulting from increasingly stringent legislation has led to the full-scale application of MBRs in Japan (Aya, 1994). In the MBR process, the cost of energy needed to maintain the cross-flow velocity and the filtration pressure is almost 90% of the total operating cost. However, using submerged membranes reduces the pumping energy requirement to 0.007 kwh/m3 of permeate (Yamamoto et al., 1989) compared with more than 3 kwh/m3 permeate required for the cross-flow mode. Table 11 presents a cost comparison of submerged MBR and conventional activated sludge processes (ASP). Based on this comparison for a small-scale wastewater treatment process, MBR systems seem to be more attractive than an ASP in terms of land and space requirements and energy consumption. Table 12 presents three different types of membrane bioreactors currently operating on municipal wastewater at semiindustrial scale plants. Here, the Renovexx process operates on settled sewage with a tabular membrane module in an external arrangement. Memcore process operates on coagulated settled sewage whereas the Kubota process works on screened sewage with a submerged membrane module system as described in Section VI. It is interesting to note that these three different MBR designs and membrane element configurations lead to the same order of magnitude of operational cost per cubic meter of treated wastewater, whereas both membrane cost and surface area requirement per cubic meter of treated wastewater is relatively large for the Kubota system.

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A. Cost Aspects of ADUF Process Strohwald (1994), cited in Ross and Strohwald (1994), carried out a capital and operating cost estimate for a 1500 m3/d ADUF system with energy recovery from the generated biogas. The design incorporated a total digester volume of 1800 m3

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TABLE 10 Operating Conditions and Performances of Anaerobic MBR Process

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TABLE 11 Comparison of Membrane Bioreactor and Conventional Activated Sludge Process


MBR (submerged type) Plant area (m2) Flow control tank ASA tanka 13.4 20.0 Activated sludge process Flow control tank ASA tankb Sedimentation tank Presediment. tank Sedimentation tank Sludge concentration tank Total Fine screen Flow control pump Flow control blower Blower for aeration 13.4 66.7 66.7 5.0 10.0 13.5

Electric power (kw)

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Total Fine screen Flow control Flow control blower Blower for aeration Suction pump Total elect. power 0.069 8.37 34.65 72% 30%

33.4 0.10 0.25 0.40 3.70 0.20 4.65

100.3 0.10 0.25 0.40 5.50

Total 0.963 11.25 48.3 100% 100%

6.25

Sludge (m3/day) Running costc ($/day) Sludge treatmentc ($/day) Running cost Space
a b c

Activated sludge aeration tank (load 2 kg/m3.day). Activated sludge aeration tank (load 0.6 kg/m3.day). Price for electricity at US$ .075 (Exchange rate of 40B/$).

From MRC, 1997.

and total MEMTUF membrane area of 1400 m2. The specific cost calculations are summarized in Table 13, assuming a 5-year depreciation and interest at 20%, based on a total capital cost for the system of 385,000. The redemption of capital is the largest cost contributing factor expected. With respect to the operating cost breakdown, a conservative 2-year membrane life was assumed for membrane replacement. The combined specific capital and operating cost of 0.04 per m3 effluent treated for a complete ADUF plant compares favorably with the cost for direct disposal of untreated effluent to municipal treatment works. The added benefit of water conservation by possible permeate increases the economic attractiveness of on site ADUF treatment.

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TABLE 12 Comparison of Operational Variables and Cost Parameters for Three Different Membrane Bioreactor Systems
Parameters Location Function Kubota Kingston Seymour, U.K. TSS, COD/BOD removal, and (de)nitrification Coated fiber Flat plate 0.4 (nominal) Screened raw sewage 6m9m 0.1 2732 125 Continuous Renovexx Newton Aycliffe, U.K. TSS, precipitated and coagulated solids removal Dynamic Al floc on substrate Tube 10 (nominal) Screened settled sewage 115 m2 (including tanks) 1 (inlet pressure 2) 110140 4000 180/25a Memcor Aberporth, U.K. TSS/BOD removal and disinfection Polypropylene HFF 0.20.3 Coagulated settle sewage 0.2 100 3750 45/2

Membrane material Membrane configuration Membrane pore size (m) Feed water specification

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Footprint Transmembrane pressure (bar) Flux (l/m2.h) Production rate (m3/day) Operation/regen. (cycle, min) Cleaning Mechanical

Water jet, 1/year

Chemical Total membrane area (m2/m3) Membrane life (years) Membrane cost (/m2) Operating cost (/m3) Replacement Chemical Other Total Capital cost (/MLD plant)
a b

2/years 1.92 ~7 80

Backwash only with water (1% of total water produced) 0.292 1.52 (w. brush cleaning) 35

Compressed air at 6 bar Every 34 d 0.72 ~5 3040

<10 10 <20 1.11.4/1

24 5 10 1721b 0.5/4

24 24 24 12 3.75

Includes membrane formation. Includes upstream chemical cost.

From Judd, S. (1998).

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TABLE 13 Specific Cost Summary of a Full-Scale ADUF Plant


Item Capital cost Investment Operating cost Electricity Membrane Maintenance Man power Total cost Subtotal (/m3) 0.282 Total (/m3) 0.282

0.023 0.042 0.026 0.021

0.112 0.394

Ross and Strohwald, 1994.

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VIII. CONCLUSION A number of full-scale MBR applications exist mostly in Japan followed by the U.S., France, the U.K., Germany, and the Netherlands. At present, the use of MBRs is reserved to situations that require good treated water quality for reuse or when stringent discharge standards cannot be technically and economically achieved by conventional effluent treatment systems (Manem and Sanderson, 1996). In the past, both capital and operational cost of membrane modules seemed to be the major hindrance to industrial-scale application of this technology. More recently, due to increased membrane production and improvement of automated systems, there has been a significant reduction in the cost of membrane systems during the last few years. Meanwhile, increasing interest in reuse of treated water and the need for more compact systems coupled with progress in research is expected to lead to more widespread application of the MBR process. Among those processes, the submerged configuration seems likely to see the widest application (Mccann, 1998). Recently, a submerged membrane system was used to upgrade existing conventional processes in two ways: (1) to increase plant capacity and (2) to improve treated water quality (Buisson et al., 1997). Given these developments and considering that, in general, membrane costs are decreasing, it can be expected that the MBR technology will become more economically competitive with conventional processes and find increasingly wider applications in wastewater treatment.

ACKNOWLEDGMENT The authors thank Terry Clayton, Centre for Language and Education Technology, Asian Institute of Technology, Thailand, for his kind assistance in reviewing and editing the final manuscript of this paper.
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