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Separation and Purification Technology 118 (2013) 89–104

Contents lists available at SciVerse ScienceDirect

Separation and Purification Technology


journal homepage: www.elsevier.com/locate/seppur

Review

A review of anaerobic membrane bioreactors for municipal wastewater


treatment: Integration options, limitations and expectations
Hale Ozgun a,b,⇑, Recep Kaan Dereli a,b, Mustafa Evren Ersahin a,b, Cumali Kinaci b, Henri Spanjers a,
Jules B. van Lier a
a
Department of Water management, Section Sanitary Engineering, Delft University of Technology, PO Box 5048, 2600 GA Delft, The Netherlands
b
Istanbul Technical University, Civil Engineering Faculty, Environmental Engineering Department, Ayazaga Campus, Maslak, 34469 Istanbul, Turkey

a r t i c l e i n f o a b s t r a c t

Article history: In recent years, anaerobic membrane bioreactor technology for municipal wastewater treatment is
Received 25 March 2013 increasingly being researched as a cost-effective alternative to produce nutrient rich, solids free effluents
Received in revised form 20 June 2013 with a high degree of pathogen removal, while occupying a small footprint. To date, especially in the last
Accepted 22 June 2013
decade, many studies have been conducted in which various types of anaerobic reactors were used in
Available online 4 July 2013
combination with membranes. This review critically evaluates the potential of anaerobic membrane bio-
reactor technology for municipal wastewater treatment with a focus on different types of anaerobic reac-
Keywords:
tors that membranes are coupled to. In addition, the paper discusses the impact of the various factors on
Anaerobic membrane bioreactor
Municipal wastewater
both biological and filtration performances of anaerobic membrane bioreactors including strengths and
Reactor membrane integration limitations.
Reuse Ó 2013 Elsevier B.V. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 90
2. Integration possibilities of membranes with different types of anaerobic reactors for municipal wastewater treatment . . . . . . . . . . . . . . . . . . . 92
2.1. Completely stirred tank reactor . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 92
2.2. High-rate anaerobic reactors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 93
2.2.1. Upflow anaerobic sludge blanket reactor . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 93
2.2.2. Expanded granular sludge bed reactor . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 93
2.2.3. Other reactor types. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 94
3. Alternative integration possibilities of AnMBRs in municipal wastewater treatment flow schemes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 94
4. Factors affecting the treatment performance of AnMBRs for municipal wastewater treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 95
4.1. Operational conditions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 95
4.1.1. Temperature . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 95
4.1.2. OLR . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 96
4.1.3. HRT . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 96
4.1.4. Upflow velocity. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 96
4.2. Sludge characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 96
4.3. Addition of adsorbents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 97
5. Factors affecting the membrane performance of AnMBRs for municipal wastewater treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 97
5.1. Membrane characteristics. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 97
5.1.1. Material . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 97
5.1.2. Module type and configuration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 97

Abbreviations: AD, anaerobic digestion; AnMBR, anaerobic membrane bioreactor; BOD, biochemical oxygen demand; CIP, cleaning in place; COD, chemical oxygen
demand; CSTR, completely stirred tank reactor; DOC, dissolved organic carbon; EGSB, expanded granular sludge bed; EPS, extracellular polymeric substances; FB, fluidized
bed; FO, forward osmosis; GAC, granular activated carbon; GLS, gas–liquid–solids; HRT, hydraulic retention time; MBR, membrane bioreactor; MF, microfiltration; MLSS,
mixed liquor suspended solids; MWC, molecular weight cut-off; OLR, organic loading rate; P/C, protein/carbohydrate; PAC, powdered activated carbon; SMA, specific
methanogenic activity; UASB, upflow anaerobic sludge blanket.
⇑ Corresponding author at: Department of Water management, Section Sanitary Engineering, Delft University of Technology, PO Box 5048, 2600 GA Delft, The Netherlands.
Tel.: +31 (0) 15 2784026; fax: +31 (0) 15 2784918.
E-mail addresses: ozgunha@itu.edu.tr, H.Ozgun@tudelft.nl (H. Ozgun).

1383-5866/$ - see front matter Ó 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.seppur.2013.06.036
90 H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104

5.2. Operational conditions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98


5.2.1. Shear rate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
5.2.2. Flux . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
5.2.3. Operation mode . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
5.2.4. Temperature . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
5.2.5. Upflow velocity. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
5.2.6. SRT. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
5.2.7. HRT . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
5.3. Sludge characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
5.4. Addition of flux enhancers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
6. Cleaning methods. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 100
7. Economic feasibility of AnMBRs for municipal wastewater treatment. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 100
8. Problems encountered and future perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 101
9. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 102
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 102
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 102

1. Introduction organic material, moderate biodegradability and its low strength


[5]. Under low temperature (<20 °C) conditions, hydrolysis of par-
Municipal wastewater is the most abundant type of wastewater ticulate matter into dissolved molecules becomes the rate-limiting
that falls into the category of low-strength waste streams, charac- step, which results in the accumulation of suspended solids (SS) in
terized by low organic strength and high particulate organic matter the reactor and a decrease in organic matter conversion efficiency
content [1]. If recoverable, municipal wastewater treatment plants together with a decrease in methanogenic activity [5,9–11]. More-
have the potential to become net producers of renewable energy, over, due to low substrate affinity of anaerobic biomass compared
converting the chemically bound energy content in the organic to aerobic bacteria it is practically very hard to achieve low efflu-
pollutants of raw municipal wastewater to useful energy carrier ent chemical oxygen demand (COD) concentrations and to fulfill
[2]. Therefore, selection of an appropriate energy recovery technol- the environmental regulations for wastewater reclamation and re-
ogy that can convert the inherent energy in wastewater into a use [12].
renewable energy source has become more important. With ever growing application experiences from aerobic mem-
Anaerobic technology has drawn considerable attention for mu- brane bioreactors (MBRs) [13], anaerobic membrane bioreactor
nicipal wastewater treatment. In addition to the energy that can be (AnMBR) technology has also started to be researched for munici-
recovered from methane-rich biogas, the application of anaerobic pal wastewater treatment as a possible alternative to the conven-
processes distinctly reduces the overall energy demand for munici- tional anaerobic treatment processes [14]. In AnMBRs, biomass can
pal wastewater treatment because no aeration energy is required be effectively retained inside the reactor providing optimal condi-
for mineralizing the organics. Moreover, anaerobic processes pro- tions for organic matter degradation without any carry-over of SS.
duce mineralized nutrients in the form of ammonia and orthophos- By incorporating membranes to anaerobic municipal wastewater
phate enabling direct agricultural use of the effluent for ferti- treatment, superior effluent quality in terms of COD, SS and path-
irrigation. The most important concern for further improving the ogen counts can be achieved in comparison with conventional
energy sustainability and resource preservation is the identifica- anaerobic processes, and a stable treatment performance can be
tion of an appropriate anaerobic technology and methods for full obtained to meet stringent discharge standards [3,15–17]. It was
recovery of the solubilized CH4 from treated effluents [2,3]. reported that AnMBRs provide a possibility for the agricultural
The retention of slow growing anaerobic biomass was the most use of the treated effluent for non-potable purposes in many re-
important challenge in the earlier development of an appropriate gions suffering from water shortage [18]. Agricultural use of trea-
reactor technology for the anaerobic treatment of municipal ted effluents generally demands extensive pathogen removal
wastewater. Treatment of municipal wastewater by different types along with the availability of macronutrients. Since macronutrients
of anaerobic processes has drawn considerable attention of various such as ammonium and orthophosphates are not removed by
researchers, e.g. [4–6]. The invention of the upflow anaerobic anaerobic bioprocesses and pathogens can be retained by the
sludge blanket (UASB) reactor in early 1970s by Lettinga and his membrane unit [19,20], permeates of AnMBRs are certainly of
colleagues was a milestone in anaerobic wastewater treatment interest for agricultural use. Information about a selected number
[7]. The major success of the UASB reactor lies in its ability to re- of guidelines on irrigation water quality can be found in the study
tain a high concentration of biomass due to formation of a thick of Norton-Brandao et al. [21]. In addition to achieving high effluent
dense sludge bed, which, in dependence to wastewater character- qualities, a shorter start-up period is required for AnMBRs in com-
istics, may consist of well settleable methanogenic sludge gran- parison to UASB systems, which is one of the major advantages in
ules. Formation of well settleable sludge allows the decoupling the treatment of especially low-strength wastewaters. Start-up
of hydraulic retention time (HRT) and sludge retention time periods of 6 and 12 days have been reported in the study of Hu
(SRT) so that efficient treatment can be carried out at high organic and Stuckey [22] and Lin et al. [23], respectively, whereas this per-
loading rates (OLRs) with a significant decrease in reactor size [4]. iod was in the range of one to several months for UASB systems
Owing to the high influent flows and low organic matter content, [24].
municipal wastewater is treated at ambient temperatures in both Despite the mentioned advantages, there are still critical obsta-
aerobic and anaerobic applications worldwide, e.g. [8], especially cles such as low flux, membrane fouling, high capital and opera-
in developing countries with (semi) tropical climates such as Bra- tional costs that limit the extensive use of AnMBRs [15,25,26].
zil, India and Colombia. However, municipal wastewater treatment AnMBRs are generally operated at higher biomass concentrations
by anaerobic systems in more temperate climates is still consid- compared to aerobic MBRs, impacting rheology and thus, reactor
ered a challenge since municipal wastewater belongs to the com- hydraulics and pumping. High mixed liquor suspended solids
plex wastewater category due to the high fraction of particulate (MLSS) concentrations also result in a more rapid and dense cake
H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104 91

Table 1
Treatment performance of membrane coupled conventional anaerobic treatment processes for municipal wastewater treatment.

Reactor type/module Volume Temperature Wastewater Influent HRT OLR SRT COD removal (%) MLSS Biogas Reference
configuration (L) (°C) source COD (h) (kg COD/ (day) (based on (g/L) production
(mg/L) m3 day) membrane (L CH4/g CODremoved)
effluent)
CSTR/side-stream 8850 25 Raw 200a 89–120 1.4–2b 144 84.5c – – [36]
CSTR/side stream 850 22 Raw 637 14.4 0.94 1 92d – 0.12 [37]
CSTR/side-stream – 25 Synthetic 500– – – 1 97 9.6– – [38]
1000 16
CSTR/submerged 3 35 Synthetic 460 3, 6, – 100 90–95 4.3– – [25]
12, 24 4.8
e
CSTR/submerged 3 35 Synthetic 465 8–20 – 250 99 2–3f – [39]
CSTR/side-stream 4 15–25 Synthetic 500 12 1 – >85 – – [17]
CSTR/submerged 6 – Synthetic 425 12 – 1g 83 4.6 – [40]
CSTR/submerged 900 – Raw 445 6–21 – 70 87 6–22 0.069 [41]
CSTR/submerged 60 30 Raw 322 10 1 1 88 6.4– 0.24 [23]
9.3
CSTR/submerged 350 35 Municipal + 630 0.8 0.6–1.1 680 90 15 0.27 [11]
glucose
CSTR/submerged 350 20 Municipal + 630 0.8 0.6–1.1 680 82–90 19 0.23 [11]
glucose
CSTR/submerged 1300 33 Pre-treated 410 6–21 0.71 76 – – – [42]
CSTR/submerged 1300 21 Pre-treated 720 6–21 0.64 74 – – – [42]
Digester/submerged 12.9 15–20 Raw 259.5 2.6 2.36 – 52–87 – – [43]
UASB/side-stream 5400 Ambient Pre-hydrolyzed 490 – 2.8b – 83 – – [44]
UASB/side-stream 34 Ambient Raw 185.6 5.5–10 0.3–0.9 1 77–81 12– 0.062– [16]
32 0.121
UASB/side-stream 15.1 35 Synthetic 150h 6 0.3i – – – – [45]
municipal
UASB/submerged 45 10–15 Raw 302.1 8 – – 56.6–57.7 5.9– – [26]
19.8f
UASB/side-stream 10 30 Synthetic 500 24 5 50 96 – – [46]
UASB/submerged 45 Ambient Raw 298.4 8 – – 63.4 – – [47]
Upflow anaerobic 180 25 Pre-settled 540 12, 6, 1.08, 1 88 14–80 – [48]
reactor/side-stream 4.5 2.16,
4.32
EGSB/submerged 4.7 11, 15, Synthetic 383– 3.5, 4.6, 1.6–4.5 145 76–96 13–23 – [49]
20, 25 849 5.7
FB reactor/– 660 – Pre-hydrolized 353 – 1.1b – 90 – – [44]
solids from
raw sewage
Hydrolyzation reactor/ 500 30 Concentrated 353 5 – – – – – [44]
side-stream solids from
raw sewage
Hydrolyzation reactor- 1000 26 Raw 2187 – – – 98 – – [50]
membrane-FB
bioreactor/side-
stream
Hydrolyzation reactor 5400 26 Raw 1144 – – – 94 – – [50]
UASB/side-stream
Jet flow anaerobic 50 37 Raw 685 15–60 0.23–2 140 88 0.5– – [51]
bioreactor/side- 10f
stream
Hybrid upflow anaerobic 17.7 Ambient Raw 97.5– 4–6 0.5–12.5 150 97 16– 0.13–0.42j [52]
bioreactor/submerged 2600 22.5
a
mg BOD/L.
b
kg BOD/m3 day.
c
VSS removal.
d
TOC removal.
e
DOC removal.
f
g VSS/L.
g
No discharge except sampling.
h
mg TOC/L.
i
g TOC/L day.
j
m3/m3 day.

layer build up in comparison to aerobic MBRs, requiring frequent Despite above constraints, AnMBR is identified as a potential
physical cleaning, interval operation, and likely sub-critical flux anaerobic process of interest for treating municipal wastewater,
operation, in order to sustain the flux [3,27–29]. Operational costs whereby, various studies indicate that treatment performances
related to energy requirements for gas/liquid recirculation for are seemingly dependent on the chosen process configuration
membrane fouling control and chemical costs required for mem- [3]. Different types of anaerobic bioreactors, including completely
brane cleaning are still heavy burdens on the economic feasibility stirred tank reactors (CSTR), UASB, expanded granular sludge bed
of AnMBRs. However, membrane acquisition and/or replacement (EGSB), etc., have been investigated in combination with various
costs have decreased significantly due to a decline in membrane types of membranes. However, the most optimal process config-
module costs [13,30,31]. uration, i.e. anaerobic bioreactor type and the coupling of the
92 H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104

bioreactor with the membrane module, yet needs to be deter- for the treatment of municipal wastewater. Tables 1 and 2 present
mined. Recently, several more general review papers on AnMBR the performance of different AnMBR applications for the treatment
systems have been published, discussing the AnMBR feasibility of municipal wastewater with regard to both biological perfor-
[32–35]. Our present paper focuses on the perspectives of the mance and membrane aspects, respectively. However, information
various types of membrane coupled anaerobic sludge bed reac- regarding the membrane performance is quite limited in most of
tors, such as UASB and EGSB, as an alternative approach to the the studies. Section 2 discusses both the advantages and disadvan-
more conventional AnMBRs consisting of CSTR type bioreactors tages of different integration possibilities of membranes with sev-
with either internal or external membrane separation devices. eral types of anaerobic reactors.
The review paper evaluates the current anaerobic bioreactor-
membrane process integration alternatives reported in the litera- 2.1. Completely stirred tank reactor
ture, with proposals for future applications. Besides, many as-
pects of current AnMBR applications for the treatment of By far, CSTR is the most common anaerobic process researched
municipal wastewater are discussed in detail including treatabil- in AnMBR systems [11,15,17,25,37–39,41] in analogy to the type of
ity and filterability. Moreover, limitations and difficulties encoun- bioreactors used in aerobic MBRs. In general, CSTRs are operated at
tered in anaerobic treatment and the possible use of the treated equal HRT and SRT without any internal biomass retention device.
municipal wastewater are discussed together with reasonable In-reactor biomass concentration can be increased by applying a
solution perspectives. secondary clarifier with return flow, resulting in an anaerobic con-
tact process, or a membrane separation device. Simple flow-
2. Integration possibilities of membranes with different types of through CSTRs, without sludge separation, are characterized by
anaerobic reactors for municipal wastewater treatment very low loading rates, resulting in long retention times and,
consequently, large reactor volumes. However, in membrane cou-
Membranes can be coupled to various anaerobic reactor types pled CSTRs, the complete retention of solids in the reactor decou-
such as CSTRs, UASB and EGSB reactors, in different configurations ples SRT from HRT, which leads to an increase in biomass

Table 2
Membrane performance of membrane coupled conventional anaerobic treatment processes for municipal wastewater treatment.

Reactor type/module configuration/ Membrane Material Pore Filtration Flux TMP Cross-flow Gas Reference
membrane configuration type size area (m2) (L/m2 h) (kPa) velocity sparging
(lm) (m/s) (L/min)
CSTR/side-stream/capillary organic – – – 7.6 – – – – [36]
membrane
CSTR/side-stream/vibratory shear – Polytetrafluoroethylene 0.45 1.59 – – – – [37]
enhanced processing (VSEP) (PTFE) Teflon
CSTR/side-stream/tubular – PTFE laminated 10 0.015 5–12 3.45–20.7 0.1–0.2 – [38]
non-woven filter
CSTR/submerged/– MF – 0.4 – 10–20 Up to 30 – – [25]
CSTR/submerged/flat sheet – Polyethylene 0.4 0.1 5–10 30–45 – 5 [39]
CSTR/side-stream/tubular MF PTFE 1 0.09 5 6.9–55.2 – – [17]
CSTR/submerged/flat sheet MF Polyolefine 0.4 0.1 10.5 – – 8 [40]
CSTR/submerged/hollow fiber – – 0.05 30 10 8 0.23a [41]
CSTR/submerged/flat sheet – Polyvinylidene fluoride 140b 0.6 12 – – 5 [23]
CSTR/submerged/flat sheet UF Polyether sulfone 0.038 3.5 7 17.7 0.026 62a [11]
CSTR/submerged/hollow fiber UF – 0.05 30 – – – – [42]
Digester/side-stream/tubular – Non-woven fabric 0.64 0.98 5 Up to 30 – – [43]
(polythylene terephthalate)
UASB/external/capillary UF Polyvinylalcohol 15b 100 – – – – [44]
UASB/side-stream/tubular – Polyacrylonitrile – 0.2 10.5 <50 0.4–1.45 – [16]
UASB/side-stream/flat sheet MF PVDF 0.22 0.05 25 30 – – [45]
UASB/submerged/flat type Dynamic Dacron mesh 61 – 65 – – [26]
UASB/side-stream/flat sheet UF PVDF coated with a 100b 0.052 8–12 – – – [46]
polyether block amide
UASB/submerged/flat sheet – Dacron mesh (dynamic 61 – 65 25 – – [47]
membrane)
Upflow anaerobic reactor/side- MF – 0.2 4 3.75, 7.50, <19.6c – – [48]
stream/hollow fiber 11.25
EGSB/submerged/hollow fiber – Polyethylene 0.1 0.1 – – – – [49]
FB reactor/external-pressure/hollow fiber MF Polyethylene 0.1 54 – – – – [44]
Hydrolyzation reactor/internal-pressure/ UF Polyacrylonitrile 13b 0.94 – – – – [44]
tubular
Hydrolyzation reactor-membrane-FB MF Polyethylene 0.1 54 24 108 1 – [50]
bioreactor/side-stream/hollow fiber
Hydrolyzation reactor UASB/side- – Polyvinylalcohol– – 100 16 147 0.7 – [50]
stream/capillary polysulfone
Jet flow anaerobic bioreactor/side- UF – 100b 1 3.5–13 100–200 3 – [51]
stream/–
Hybrid upflow anaerobic bioreactor/ – Polyethylene 0.03 0.3 5–10 <70 – – [52]
submerged/hollow fiber
a
m3/m2 h.
b
kDa, molecular weight cut off.
c
Driven by water level difference.
H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104 93

concentration and thus increase in conversion rates alleviating the biological processes take place inside the dense sludge bed in the
rate limiting step, e.g. hydrolysis/solubilization of solids and/or bottom of the UASB reactor [55]. The physical removal of particu-
methanogenesis. Often CSTRs are coupled to external cross-flow late organics by settling, adsorption and entrapment in the sludge
membranes, resulting in high bioreactor liquid turnover rates, bed of the UASB makes it appropriate for the first treatment step of
leading to a well-mixed flow regime. In addition, as a result of municipal wastewater, which is generally characterized by a high
the prevailing high shear stress and intense mixing, an AnMBR particulate COD/soluble COD ratio. In fact, UASB reactors can be
set-up might even increase the biological methane potential of upfront used as biofilters before membrane treatment, which pre-
the substrate [3]. vents the membrane from excessive exposure to high SS concen-
Notwithstanding its advantages, CSTRs directly expose the trations. For instance, while a UASB reactor had a biomass
membrane to bulk sludge, which results in heavy membrane foul- concentration of 20–30 g/L, SS concentration in the effluent was
ing and low fluxes since effluent solids concentration of CSTRs is below 1 g/L [56]. An et al. [16] reported TSS concentrations in the
equal to the bulk solids concentration [3]. The high solids concen- range of 11–32 g/L in a UASB reactor; whereas, total solids (TS)
tration subjected to membrane filtration exacerbate cake deposi- concentration in the effluent was less than 50 mg/L. Obviously,
tion in CSTR configuration, either with pressure-driven or the efficiency of solids entrapment determines the amount and
vacuum-driven membranes. Moreover, sludge recirculation properties of solids leaving the UASB with the effluent. In this con-
through the membrane feed pump, especially for external cross- text, HRT and upflow velocity in membrane coupled UASB reactors
flow membranes, results in a substantial decrease in the mean par- seem to be the critical parameters determining the efficiency and
ticle size [53]. On one hand, disruption of particles may positively effluent fouling propensity. High SRTs and OLRs can be maintained
impact hydrolysis, but on the other hand it may negatively impact by applying UASB reactors, without increasing the effluent solids
the juxtapositioning of acetogens and methanogens, limiting the concentration that will be subjected to membrane filtration. Thus,
required interspecies hydrogen transfer for attaining a high spe- membrane flux may become less dependent on the reactor MLSS
cific methanogenic activity (SMA) [54]. concentration, possibly leading to high membrane fluxes. There
Martinez-Sosa et al. [11] studied an AnMBR system consisting of are many studies that focus on the fouling potential in AnMBR sys-
an external ultrafiltration (UF) membrane coupled to a CSTR for the tems including UASB reactors coupled to membranes. Liao et al. [3]
treatment of municipal wastewater and obtained an effluent that suggested that membrane coupled UASB systems may decrease the
can be used for agricultural irrigation. An innovative process, i.e. capital cost of UASB reactors by eliminating the need for a gas–li-
vibrating membranes coupled to a CSTR, was proposed by Grunde- quid–solids (GLS) separator in a UASB. Moreover, organic fouling
stam and Hellstrom [37] for the treatment of municipal wastewa- may be reduced by increasing the SRT which leads to high biomass
ter. They achieved high total organic carbon (TOC) removal concentrations in the reactor and, through increased entrapment in
efficiency of 92%. Authors subsequently applied reverse osmosis the bed, lower COD concentrations in the effluent of the UASB reac-
(RO) as post-treatment in order to concentrate the nutrients for tor [3]. Obviously, with increased biogas production the absence of
further use on agricultural lands. Ho and Sung [17] reported a GLS separator will likely lead to high sludge carry over to the
high COD removal efficiencies for membranes coupled CSTRs effluent.
treating synthetic municipal wastewater. Gimenez et al. [41] Despite the expected more efficient membrane filtration step,
tested hollow fiber membranes in an AnMBR system consisting for the treatment of municipal wastewater under sub-mesophilic
of a CSTR and submerged membranes immersed in an external conditions, hydrolysis of the retained particulates likely becomes
chamber and achieved a COD removal efficiency of 90% with a flux the rate-limiting step and particulate matter accumulation in the
of 10 L/m2 h. sludge bed will occur, subsequently resulting in activity loss [5].
Furthermore, a thinner and less porous cake layer on the mem-
2.2. High-rate anaerobic reactors brane surface can be expected, possibly leading to more serious
pore clogging problems in UASB coupled AnMBRs, since the mem-
In high-rate anaerobic reactors such as sludge bed systems and brane would be exposed directly to only fine particles instead of a
anaerobic filters, biomass is retained either by the formation of range of particle sizes. According to the previous results particu-
granular and/or thick flocculent sludge or by attachment to a sup- larly the small (submicron) particles determined the operational
port material. Effluent SS concentration is significantly lower than flux [57,58]. Therefore, the degree of small particle retention by
the biomass concentration in the reactor, which makes them feasi- the sludge bed will be of prime importance for the feasibility of
ble for high hydraulic loadings. For instance, sludge bed systems coupled membrane filtration.
are characterized by total suspended solids (TSS) concentrations In some studies, researchers used membrane filtration as a
ranging between 20 and 40 kg/m3 reactor volume [55]. As in these polishing step after UASB systems without returning the
reactors biomass is not directly subjected to membrane filtration, concentrate stream to the bioreactor as it is applied in AnMBRs
dense cake layer formation and consolidation will be less apparent [12,59–61] (Fig. 1). These configurations can be regarded as
in comparison with CSTRs when combining these reactors with a tertiary filtration. This approach has the advantage of easier
membrane module. Therefore, high rate anaerobic reactors may of- control of hydraulics in the UASB reactor and the preservation
fer a good opportunity for being combined with membranes, espe- of the dilution rate as bacterial selection criterion. However, it
cially if very low SS concentration is required in the effluent and may have the disadvantage of high SS concentrations exposure
retention of biomass is required under presence of toxicity related to the membrane because SS would be concentrated in the
to discharges of industrial wastewater in the municipal sewer sys- concentrate collection tank.
tems, or hydraulic overload events [3]. However, the impact of
membrane application on sludge immobilization and granule sta- 2.2.2. Expanded granular sludge bed reactor
bility is not yet well understood. UASB reactors treating sewage at low and moderate tempera-
tures are sometimes characterized by a poor mixing regime, which
2.2.1. Upflow anaerobic sludge blanket reactor causes a decrease in soluble COD treatment efficiency. To solve this
UASB reactors coupled to membrane separation can be a rea- problem, tall reactors with a small footprint and external or inter-
sonable option to decrease the SS concentration being sent to the nal effluent recirculation are being applied, i.e. the so-called EGSB
membrane since the sludge bed would entrap most of the particu- reactors [62]. Bench scale and (semi-)pilot studies have shown that
late matter by adsorption and biodegradation [16,44,45,47]. All an EGSB reactor is an attractive alternative, especially for the
94 H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104

3. Alternative integration possibilities of AnMBRs in municipal


wastewater treatment flow schemes

In view of cost-effective municipal wastewater treatment,


which also aims at recovery of resources (nutrients), production
of energy, and the use of the treated effluent, integrated system ap-
proach deserves more attention than solely the coupling of a spe-
cific anaerobic reactor type to membrane units. By that approach,
the optimum way of closing nutrient and water cycles should be
determined. Some alternative integration options for AnMBRs in
conventional wastewater treatment schemes can be found in the
literature. However, innovative possibilities should be continu-
Fig. 1. Membrane filtration used as a post-treatment step after UASB reactors.
ously developed for energy and nutrient recovery.
For municipal wastewater treatment at low (15 °C) and/or
fluctuating temperatures (15–25 °C), a two-step system including
treatment of low strength wastewaters at ambient temperatures, a UASB reactor combined with an additional sludge digester was
due to the efficient biomass–substrate contact induced by the shown advantageous to prevent activity loss in the sludge bed
applied high upflow velocity [63–65]. Besides, higher OLRs can due to slowly degradable particulate matter accumulation [66].
be applied in EGSB reactors compared to UASB reactors. However, In this system, the non-degraded particulate COD entrapped in
SS are limitedly removed from the wastewater and sludge washout the sludge bed of the UASB reactor is further stabilized in a sepa-
would occur in the system due to high upflow velocity. Therefore, rate CSTR type digester operated under optimal mesophilic condi-
anaerobic treatment applying EGSB systems is restricted to pre- tions (30–35 °C). The UASB-Digester set-up is proposed to
settled sewage only. As an alternative to pre-settling, Chu et al. overcome the hydrolysis limitation induced by low temperatures
[49], as the sole example in literature, proposed a membrane unit and to reduce non-stabilized particulate matter accumulation in
that is capable of retaining the SS inside the EGSB reactor. In that the sludge bed. By recirculating the digested solids to the UASB
study, the membrane module is submerged in the upper part of reactor, the sludge bed SMA is increased resulting in enhanced re-
the EGSB reactor and the applied high upflow velocity was moval of soluble organics [66]. Membrane integration to the UASB-
beneficial in the reduction of membrane fouling due to the Digester system can be attractive for producing high quality and
increased hydraulic shear stress on the membrane surface [49]. nutrient-rich effluents for reuse purposes under moderate climate
Nonetheless, cake layer resistance governed the achievable flux conditions (Fig. 2a).
over the hollow fiber membranes, whereas pore blocking only Since anaerobic processes are particularly of interest for con-
was of minor importance. Based on the high removal efficiencies centrated waste stream, upconcentration of sewage using forward
even at low temperatures, the use of EGSB reactors in AnMBRs osmosis (FO) technology is currently receiving increasing interest
was suggested as a potential technology for treating municipal [67]. FO uses an osmotic pressure gradient to drive water across
wastewater at ambient temperature [49]. Following their reason- a semi-permeable membrane from the low osmotic pressure side
ing, submerged membrane configurations are found more appro- (feed solution) to the high osmotic pressure side (draw solution).
priate than external configurations for the use of EGSB reactors Owing to the absence of pressure driven water transport, FO mem-
in AnMBRs. However, membrane integration eliminates the branes are not susceptible for the traditional sewage fouling pro-
hydraulic selection pressure required for granulation, by avoiding pensities [67,68]. FO processes may be used as a pretreatment to
the wash out of flocculent sludge with poor immobilization charac- concentrate municipal wastewater in coastal areas where the sea
teristics. Therefore, no granulation is expected in EGSB reactors water can be used as a draw solution [67,69]. Alternatively, closed
coupled to membrane filtration, which would decrease the settlea- loop draw solutions can be used, however, at the expense of energy
bility of the biomass on the long term operation. consumption for draw solution regeneration. For the optimization
of energy and other operational costs, appropriate draw solutes
2.2.3. Other reactor types and concomitant regeneration methods are being researched
In addition to the most popular high rate reactors, i.e. UASB [70,71]. A decrease in wastewater flow is regarded as the benefit
and EGSB reactors, other reactor types such as hybrid upflow of the FO based concept resulting in small treatment systems with
anaerobic systems [52] and jet flow anaerobic reactors [20] were anaerobic digestion (AD) as the main bio-stabilization process
also used for the treatment of municipal wastewater at low [67,72]. A possible integration of the FO unit in an AnMBR treat-
temperatures. ment system is given in Fig. 2b. Interestingly, a current Dutch pro-
Wen et al. [52] operated a hybrid upflow anaerobic system cou- ject researches the possibility to extract fresh water from sewage
pled to a membrane unit for 200 days. The hybrid system consisted using FO, whereas the AD-recovered energy from the concentrated
of an anaerobic bioreactor column in which the bottom part was sewage is used for re-concentrating the draw solution. The energy
used as a sludge bed zone and the upper filter part was packed needed for the desalination part of the total process could be ob-
with fine fibers to prevent sludge washout. They obtained a high tained by digestion of the concentrated sewage. However, further
COD removal efficiency (>97%) with an effluent COD concentration research should be done in order to clarify the sufficiency of the
up to 20 mg/L. It was also reported that high OLRs (0.5– produced energy to drive the whole integrated concept [73].
12.5 kg COD/m3 day) could be applied successfully. Due to the low COD concentrations and concomitant high influ-
A jet flow anaerobic reactor [20] was coupled to membrane fil- ent flow rates, high membrane surface areas and/or high fluxes are
tration for the treatment of municipal wastewater. Circulation of required for municipal wastewater treatment, using membrane
the liquid inside this type of reactor by using an inner tube and a technology. Therefore, a pretreatment step such as (advanced) so-
nozzle system provides a good homogenization inside the reactor. lid/liquid separation in municipal wastewater is of interest when
By using an UF membrane coupled to the jet flow anaerobic reac- AnMBR systems are considered for municipal wastewater treat-
tor, total removal of pathogens and high quality effluent were ob- ment. Consequently, AnMBRs may take the role of sludge digesters
tained of interest for agricultural usage [20]. in municipal wastewater treatment systems as presented in Fig. 2c.
H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104 95

(a) (b)

(c) (d)
Fig. 2. Alternative integrated flow schemes of AnMBRs.

A similar flow scheme was proposed by Sutton et al. [74]. The latter membrane units. The membrane coupled FB reactor was operated
authors carried out a model based feasibility study with mass bal- at an OLR of 1.1 kg biochemical oxygen demand (BOD)/m3 day
ance calculations for a conceptual flow diagram of a municipal with 91% BOD removal.
wastewater treatment plant consisting of aerobic and anaerobic In case nutrient removal is required instead of recovery for re-
MBRs and innovative nutrient recovery processes such as ammonia use, all proposed flow schemes can be modified by adding innova-
removal by using zeolite, and orthophosphate removal by a reactive tive nutrient removal systems such as Sharon/Anammox [76,77]
filtration system. They proposed to shuttle the largest fraction of or- and struvite recovery [78,79]. Grundestam and Hellstrom [37] pro-
ganic carbon in the wastewater into solids slurry and to further di- posed to treat AnMBR effluents by RO membranes in order to
gest the organic solids in an AnMBR. Modeling and simulation achieve high nutrient recovery and water reuse. The system was
results were used to optimize the design of the system with respect operated at 22 °C without any heating and a high permeate quality
to energy usage and solids production and to obtain cost savings. was obtained. Removal efficiencies obtained by the proposed sys-
Minimization of residual solids production and maximization of tem were 91%, 99% and >99% for Kjeldahl nitrogen, phosphorus
the energy produced resulted in cost reduction. However, results and TOC, respectively. Total energy consumption of the system
are theoretical and emphasis should be given to membrane perfor- was reported as 3–6 kW h/m3.
mance, validating the concept with pilot and full scale studies.
Another alternative for AnMBR integration as a sludge digester
4. Factors affecting the treatment performance of AnMBRs for
is depicted in Fig. 2d. The main difference between Fig. 2c and d is
municipal wastewater treatment
the presence of a membrane coupled hydrolysis reactor in Fig. 2d.
The hydrolysis reactor can be used for solubilization of particulate
Optimization of AnMBR processes generally focus on either the
organic matter which may accumulate in the UASB reactor. The
improvement of biological efficiencies, e.g. [80] or on enhancing
generated volatile fatty acids (VFAs) can be further converted to
the membrane based separation process [81,82]. Few authors re-
methane in a subsequent high rate anaerobic system such as mem-
search the interaction between both processes [39,49]. In subse-
brane coupled UASB reactor or can be used for other purposes. This
quent paragraphs the impact of the various factors, including the
approach was investigated at pilot scale by Kiriyama et al. [36,75]
key operational parameters such as temperature, HRT, upflow
who concentrated raw sewage by a filter unit and fed the thick-
velocity, OLR as well as sludge characteristics, and addition of
ened sludge to a hydrolysis reactor equipped with external cross-
adsorbents, on both biological and physical aspects are further
flow membranes. Volatile suspended solids (VSS) reduction rate in-
discussed.
creased from 45% to over 80% by the addition of a membrane mod-
ule to the hydrolysis reactor. The pre-acidified wastewater was
further treated in a UASB reactor. However, no information about 4.1. Operational conditions
the membrane performance was given in the study. Kataoka
et al. [44] operated a two stage system consisting of a hydrolysis 4.1.1. Temperature
reactor and a fluidized bed (FB) reactor for the treatment of muni- The temperature dependence of biological reaction rates car-
cipal wastewater. Both reactors were equipped with external ries vital importance for the overall efficiency of a biological
96 H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104

treatment process. Generally, the activity of microorganisms in a 4.1.3. HRT


biological process decreases when the temperature decreases, HRT is an important parameter from an economic perspective
which consequently results in a decrease in COD removal efficien- as it has a strong influence on capital costs, considering that short-
cies. Besides its effect on the metabolic activities of the microbial er HRTs allow smaller reactors [12]. Therefore, the influence of HRT
population, temperature has a profound effect on factors such as on the biological removal efficiency of AnMBRs treating municipal
biogas solubility, solubility of (in)organic compounds, and the set- wastewater has been investigated by various researchers. Among
tling characteristics of the biological solids due to water viscosity them, Hu and Stuckey [25] studied an AnMBR operated at 35 °C
changes [83]. and concluded that COD concentrations both in the reactor and
Chu et al. [49] investigated the effect of temperature on the per- permeate increased slightly with a decrease in HRT due to an in-
formance of membrane-coupled EGSB reactor at moderate and low creased organic load. Chu et al. [49] also studied the effect of
temperatures. Temperature strongly affected the rate of the anaer- HRT at various temperatures on the treatment performance of a
obic conversion process and a decrease in both COD removal effi- membrane-coupled EGSB reactor. They found that COD removal
ciency and activity was observed with the decrease in efficiency was independent of HRT at temperatures higher than
temperature from 25 °C to 11 °C. However, the contribution of 15 °C. However, an increase in COD removal efficiency was ob-
the membrane to the COD removal efficiency increased from served with an increase in HRT at 11 °C, indicating the significance
8.8% to 14.2% with the decrease in temperature, which demon- of HRT at low temperatures. HRT was controlled as an independent
strated the advantage and robustness of membrane-coupled reac- parameter from upflow velocity in the study of Chu et al. [49] by
tors in maintaining high treatment efficiency even at low introducing effluent recirculation to the reactor. However, for up-
temperatures due to the complete retention of particulate COD flow reactors without recirculation, effects of HRT and upflow
and biomass. This is in agreement with findings of Ho and Sung velocity can be evaluated dependently as they are inversely pro-
[17] who also investigated the effect of temperature in the treat- portional to each other as in the study of An et al. [16]. They re-
ment of municipal wastewater by AnMBRs. Two identical AnMBRs ported an increase in the TOC removal efficiency when the HRT
were operated at 25 °C and 15 °C in parallel for 112 days. They re- of a membrane coupled UASB reactor was decreased from 10 h to
ported that the physical removal capacity by the membrane com- 5.5 h. They explained this as a result of improved wastewater dis-
pensated for the decreased SMA and biological removal rate at tribution in the sludge bed and better contact between biomass
15 °C by rejecting soluble organics. Wen et al. [52] also observed and substrate at higher upflow velocity. Based on the results, it
that AnMBRs treating municipal wastewater had a strong tolerance can be hypothesized that there is an optimum HRT for each case,
to temperature fluctuations between 12 °C and 26 °C. They ob- which is determined by many factors such as system hydraulics,
tained 88% COD removal even at 12 °C. Martinez-Sosa et al. [11] re- wastewater characteristics and sludge properties, to provide both
ported that bioreactor temperature impacted methane recovery in efficient biological removal and filtration performance.
an anaerobic externally submerged MBR treating municipal waste-
water. COD removal efficiencies close to 90% were achieved at both 4.1.4. Upflow velocity
35 °C and 20 °C. A stable cake layer formation on the membrane Upflow velocity is an important parameter having two oppos-
surface may compensate differences in biological organic matter ing effects on the biological removal efficiency in upflow reactors.
degradation rate at different temperatures. Although CH4 recovery An increase in upflow velocity may enhance mixing providing
at 20 °C is lower owing to the higher solubility of CH4 at lower tem- better substrate–biomass contact. On the other hand, increasing
peratures, interestingly, the methane content of the biogas was upflow velocity may deteriorate the removal efficiency by exceed-
higher at low temperatures due to the gas solubility difference of ing the settling velocity of particles, resulting in the detachment
CO2 and CH4 at 20 °C compared to 35 °C. Lower solubility of meth- of the captured solids due to high hydraulic shear force [84]. Dif-
ane in comparison to CO2 at 20 °C resulted in a major proportion of ferent upflow velocities were applied in Chu et al.’s [49] study by
CO2 in the liquid phase leaving the reactor and an increase in the using effluent recirculation in a membrane-coupled EGSB reactor
proportion of methane from 80% to 88% in the gas phase. Gimenez and a better COD removal performance was achieved at higher
et al. [42] also investigated the effect of temperature on methane upflow velocities which supported the former hypothesis of Mah-
recovery efficiency in an AnMBR system treating municipal waste- moud et al. [84]. Besides, a significant increase in COD removal
water. They obtained slightly lower values at 20 °C in comparison efficiency was observed with an increase in upflow velocity at
to 33 °C due to a reduction in the treatment efficiency and an in- 11 °C in comparison with a slight increase at 25 °C, which demon-
crease in the gas solubility. strated the importance of adequate hydraulic mixing at lower
temperatures.

4.1.2. OLR 4.2. Sludge characteristics


AnMBR processes have the advantage of tolerating changes in
organic loading similar to its tolerance to the fluctuations in tem- Biomass characteristics, bacterial flora, e.g. the fraction of slow-
perature. OLRs ranging from 0.3 to 12.5 kg COD/m3 day have been growing bacteria, and nutritional requirements, are mainly depen-
applied in AnMBRs treating municipal wastewater (Table 1). Wen dent on the type and operational conditions of bioreactors [44].
et al. [52] confirmed that an excellent effluent quality could be ob- There are several reports asserting an activity loss of biomass,
tained by the combination of an anaerobic bioreactor with a mem- especially of propionate degraders, in AnMBRs [54,85]. This may
brane unit in spite of high OLR fluctuations between 0.5 and be due to lysis of the cells under high shear or disruption of
12.5 kg COD/m3 day, which generally would cause perturbations juxta-positioning of the hydrogen producing bacteria and
in conventional anaerobic reactors. Accordingly, Lin et al. [23] ob- hydrogenotrophic methanogens, enlarging the interspecies hydro-
served relative stability in the permeate COD regardless of the fluc- gen transfer distance. On the other hand, Jeison et al. [58] pre-
tuations in the influent COD. The quality of the effluent was also served both methanogenic and acetogenic activities in a cross-
stable in the study of An et al. [16] in spite of the fluctuations in flow AnMBR system applying liquid superficial velocities of 1–
OLR. They stated that AnMBR could achieve more stable effluent 1.5 m/s and gas slug upflow velocities of 0.1 m/s. SMAs of the
quality in comparison to a conventional anaerobic process. More- cross-flow AnMBR sludge using propionate as the substrate were
over, it was shown that the biogas yield increased linearly with even higher than those of a parallel operating UASB system. Other
an increase in the organic loading. studies focus on differences in microbial species composition or
H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104 97

activity profiles between the fouling layer and biomass suspension 5.1. Membrane characteristics
of AnMBRs treating domestic sewage [17,46]. Ho and Sung [17]
found that SMA of the biomass attached to the membrane surface 5.1.1. Material
was lower compared to the bulk sludge in an AnMBR treating mu- Membrane material characteristics may affect the degree of
nicipal wastewater. Thus, the attached sludge did not play a signif- fouling in AnMBRs; e.g. organic and inorganic membranes may
icant role as a biofilm for biological removal compared to show different fouling behaviors. Kang et al. [88] reported that
suspended sludge. Zhang et al. [47] also investigated the character- cake layer formation was the main mechanism for fouling of or-
istics of the fouling layer and the bulk sludge in a dynamic AnMBR ganic membranes, whereas inorganic precipitation, mainly stru-
system in which separation is achieved by a dynamic cake layer vite, played the key role in the fouling of inorganic membranes.
that is formed by bulk sludge. Microorganism communities were Gao et al. [46] observed differences in fouling rates and foulant
found to be different from the bulk sludge, and activity of microor- layer composition even for two different organic membrane mate-
ganisms in the dynamic cake layer was found lower than bulk rials. They found that fouling of uncoated polyetherimide (PEI) UF
sludge due to the compactness of cake layer which resulted in sup- membranes occurred faster than polyvinylidene fluoride (PVDF) UF
pressed mass transfer. membranes coated with polyether block amide, reaffirming the
Lin et al. [23] investigated the effect of sludge concentration on significance of membrane material on fouling. Furthermore, they
biological treatment of AnMBRs and observed a relative stability in determined significant differences in bacterial composition in the
the permeate COD regardless of the fluctuations in sludge concen- fouling layers of different membrane materials. Although Bacteroi-
trations between 6.4 and 9.3 g MLSS/L. detes were absent in the fouling layer of PVDF membrane, they
were present on PEI membrane. Observations of Gao et al. [46]
show that membrane material may affect the interactions between
4.3. Addition of adsorbents different microbial species and membrane surface, and thus the
fouling phenomena, and support the value of integrating mem-
PAC and zeolites can be added into AnMBRs in order to adsorb brane material science with deep understanding of the adhesion
soluble organic compounds. By this way, these materials reduce or- and biofilm-formation potential of different microbial species.
ganic fouling, enhance membrane flux and also affect biological
treatment performance [86]. Hu and Stuckey [25] investigated
the effect of both PAC and GAC addition on the performance of 5.1.2. Module type and configuration
AnMBRs. The addition of PAC resulted in a significant increase in Various membrane configurations such as flat sheet, hollow fi-
COD removal efficiency, whereas only limited effect was observed ber, and tubular membranes are applied in AnMBRs, using different
after GAC addition. This was attributed to the larger surface of PAC types of module configurations such as submerged/immersed and
per unit mass compared to GAC, thus more colloids and macromol- external cross-flow systems [3]. Submerged AnMBRs can also be
ecules could attach to PAC from the bulk solution. VFAs were only used in different configurations including directly immersed into
limitedly absorbed to the activated carbon. Interestingly, the SMA the bioreactor or immersed in a separate membrane tank. Gener-
of the sludge growing in the AnMBR without activated carbon ally, for submerged AnMBRs flat sheet and hollow fiber mem-
addition was lower compared to that from the AnMBR with acti- branes are preferred, whereas external cross-flow AnMBRs can be
vated carbon addition. This finding was explained by the support configured with tubular membranes as well [3]. Different hydrody-
surface provided by activated carbon in order to protect the bio- namic conditions in submerged and external cross-flow AnMBRs
mass from high shear conditions. Besides, Vyrides and Stuckey have different effects on the bulk sludge properties, attainable flux
[39] observed an increase in dissolved organic carbon (DOC) re- and membrane fouling due to the extent of applicable shear rate
moval after the addition of PAC due to the adsorption of high [89]. AnMBRs configured with external cross-flow membranes
molecular weight compounds. may provide a higher flux [90] and need a lower membrane area
in comparison to their submerged counterparts. However, energy
required for the cross-flow pumps would be high due to the high
5. Factors affecting the membrane performance of AnMBRs for flow to be pumped for providing enough hydraulic shear force.
municipal wastewater treatment Martin-Garcia et al. [91] compared specific energy demands for dif-
ferent configurations of AnMBR treating municipal wastewater and
Flux decline, especially in long-term operation, seems to be found that 0.3 kW h/m3 permeate and 3.7 kW h/m3 permeate were
the most critical constraint for the applicability and feasibility needed for submerged and external cross-flow configurations,
of AnMBRs for municipal wastewaters, since it plays a major role respectively. The amount of pumping energy may be decreased
in the determination of the required membrane area. A number of by using small diameter tubular membranes since the packing area
factors are associated with flux decline. Therefore, the research of of the membrane module can be increased. On the other hand, high
membrane fouling behavior and mechanisms requires the under- hydraulic shear force may also disrupt anaerobic biomass and gen-
standing of several factors such as membrane characteristics, erate small particles, which result in significant membrane fouling.
operational conditions and sludge properties. So far, membrane Besides, biological activity of anaerobic biomass may decrease due
fouling in AnMBRs has not been fully understood due to the com- to the high hydraulic shear force [92].
plex nature of membrane foulants and diversity of operational An et al. [16] investigated the effect of different tubular mem-
conditions, membrane materials, configurations and wastewaters brane diameters, i.e. 3.0, 1.9, 1.2 mm, on the filtration performance
in different studies. Multiple and complex interactions occur be- of an external cross-flow AnMBR treating municipal wastewater.
tween physical and biological factors not only in real plants but The results showed that the variations of TMP were reciprocally
also in controlled lab-systems. Therefore, fouling phenomena correlated with the variations in tube diameter. This phenomenon
should be investigated under well-defined combinations of was related to the particle accumulation that occurred in the lu-
parameters and conditions which individually might even present men. A smaller diameter tube was simply blocked by large parti-
opposing effects [87]. Having outlined the key parameters affect- cles, which caused serious membrane clogging in comparison to
ing biological treatment performance, major factors that affect fil- the tubes with larger diameter. The blockage of small diameter
terability in AnMBRs for municipal wastewater treatment will tubes resulted in an uneven flux distribution along the membrane
now be discussed. module and an increase in the local flux, which finally caused more
98 H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104

serious membrane clogging in comparison to the tube with larger 5.2.3. Operation mode
diameter. The operation mode of membrane systems is another important
factor influencing fouling in AnMBRs. Generally, backwashing and/
or relaxation are used as strategies to decrease fouling. Moreover,
5.2. Operational conditions
optimization of backwash and relaxation duration and/or fre-
quency plays an important role in flux enhancement. Lew et al.
5.2.1. Shear rate
[48] emphasized the necessity of backwash frequency optimiza-
Removing the deposited cake layer from the membrane surface
tion for fouling reduction. They obtained similar fouling rates for
is very important to achieve a steady operation in AnMBRs. Cross-
15 and 30 min backwash frequencies; however, higher fouling rate
flow and biogas sparging may be regarded as principle mecha-
was observed at a higher backwash interval of 60 min. Chu et al.
nisms to provide shear over the membrane surface in order to limit
[49] also dealt with finding optimal operating modes and observed
the deposition of particles and restrict their interaction with the
an increase in permeability and enhancement in the permeate flux
membrane [3]. The cake layer formation rate was found to be pos-
recovery with increasing relaxation time. During the relaxation
itively correlated with the fraction of small size particles and flux,
period, efficient cake layer removal from the membrane surface
whereas it was negatively correlated with shear rate [92].
was achieved. Gimenez et al. [41] operated a pilot scale AnMBR
Although, increasing shear rate can help to reduce fouling and cake
equipped with hollow fiber membranes for the treatment of muni-
resistance, and improve flux, there appears to be a certain limit for
cipal wastewater and obtained a flux of 10 L/m2 h at an MLSS con-
both cross-flow velocity and gas sparging rate beyond which it
centration of 22 g/L. They prevented fouling with the help of a
would practically have little or no added benefit. Choo et al. [93]
rather complex membrane operation mode including backwash,
indicated that cake layer resistance can be decreased by increasing
relaxation and degasification cycles. An et al. [16] compared back-
cross-flow velocity. However, at a Reynolds number of 2000, a pla-
wash, relaxation and continuous filtration modes and maintained
teau was reached and no further reduction in the resistance could
low TMP for a longer time in backwash mode in comparison to
be obtained. The same is true for the gas sparging rate. Xie et al.
relaxation or continuous filtration modes.
[94] reported that the critical flux of a submerged AnMBR in-
creased and the fouling rate decreased when the biogas sparging
5.2.4. Temperature
rate was increased from 10 to 25 L/m2 min. However, they indi-
Temperature affects not only the rate of the biodegradation pro-
cated that there was a practical limit above which further increas-
cess but also the viscosity of the filtered liquid and the solubility of
ing the biogas sparging rate provided little added benefit. Similar
various compounds and gases. Since under practical conditions
results, also for submerged AnMBRs, were presented by Jeison
sewage temperatures cannot be altered, the operational tempera-
and van Lier [28].
ture is of significant importance for municipal wastewater treat-
Moreover, high shear rates may also stimulate the break-down
ment using AnMBRs. Martinez-Sosa et al. [11] stated that the
of microbial flocs and increase the cake layer resistance due to the
operational temperature of an AnMBR is related to the observed
selective deposition of fine particles in the cake layer and mem-
membrane fouling. Although they operated the system at a flux
brane pores during long term operation. This results in the forma-
of 7 L/m2 h at 35 °C, they observed an increase in the fouling rate
tion of a dense consolidated cake layer that is very hard to remove.
at 20 °C, possibly due to TSS and soluble COD accumulation and
This phenomenon has been called as the shear rate dilemma [57].
a higher viscosity in the bioreactor. Decrease in temperature and
An et al. [16] investigated the effect of cross-flow velocity on foul-
increase in solids content were proposed as possible explanations
ing in a UASB reactor equipped with tubular membranes. They
for viscosity increase. The fouling rate was reported as
concluded that a low TMP can be maintained for a long time at
0.14 mbar/d at 35 °C, whereas it was 2.61 mbar/d at 20 °C.
high cross-flow velocities. However, this operation condition led
to a high irreversible fouling due to the deposition of small sized
5.2.5. Upflow velocity
particles on the membrane surface and inside the pores during
The upflow velocity in (submerged) AnMBRs generally has a po-
long term operation.
sitive impact on filterability mainly due to increased shear stress.
Duration and frequency of applied shear rate may also have an
Chu et al. [49] operated an EGSB reactor equipped with a sub-
effect on filterability. Vyrides and Stuckey [39] reported that
merged membrane module and observed an increase in permeabil-
switching from continuous biogas sparging to intermittent mode
ity with the increase in upflow velocity likely due to the shear
(10 min ON/5 min OFF) resulted in a small increase in TMP. How-
effect of higher upflow velocities. However, on the long term, a flux
ever, it improved the DOC removal of submerged AnMBR due to
decline was observed indicating a decreased contribution of up-
the formation of a thicker cake layer on the membrane surface. Un-
flow velocity to fouling control, suggesting the inadequacy of shear
der these conditions a higher rate of biodegradation was observed
force induced by high upflow velocity to combat cake layer forma-
because the substrate was in contact with a thicker biofilm and
tion. Possibly, the observed phenomenon can be attributed to
more of the higher molecular weight solutes were retained until
strong adhesion of the foulants to the membrane surface and an in-
they could be degraded.
creased thickness of the cake layer.

5.2.2. Flux 5.2.6. SRT


Choice of the operational flux is very important in terms of foul- SRT has been identified as the main parameter influencing flux
ing management. Operation below the critical flux, which depends with values typically dropping at higher SRTs. Operation of anaer-
on membrane characteristics, operating conditions and sludge obic systems at ambient temperatures becomes feasible only if SRT
characteristics, is an effective approach to avoid severe fouling is approximately twice as high as that under mesophilic conditions
within a filtration system [95,96]. Martinez-Sosa et al. [18] re- [97]. As a rule of thumb, SRT should be at least three times the dou-
ported that an AnMBR treating municipal wastewater could be bling of the slowest growing organism responsible for bioconver-
operated stable for a long time at a critical flux of 7 L/m2 h with sion [55]. High capability of solids retention in membrane
a biomass concentration of 14.8 g TSS/L and a gas sparging velocity systems makes membranes ideally suited for anaerobic treatment
of 62 m/h. Increasing flux to 10 L/m2 h and 12 L/m2 h resulted in an of municipal wastewaters especially at low temperatures when the
unstable operation due to the high fouling rate that could not be degradation rate of SS and colloidal materials is the rate limiting
controlled even at higher gas sparging velocities. step [26]. Since the particulate organics would also be retained in
H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104 99

the reactor, they can eventually be further hydrolyzed and de- [60] study. High molecular weight SMP was associated with long
graded [26]. However, although membrane processes result in sol- SRT, incomplete organic matter hydrolysis and rate limitations of
ids retention independently of temperature [3], the activity anaerobic microorganisms at low temperatures, e.g. 20 °C. Low
limitation of anaerobic microorganisms at low temperature might molecular weight SMP have the propensity to pass freely through
yield high colloidal and soluble solids in anaerobic effluents, result- membrane pores. However, it can also adsorb onto the membrane
ing in an increase in membrane fouling propensity [60]. SRT of surface leading to an intermediate blocking or deposit inside the
more than 140 days was reported as a possible cause of severe pores resulting in standard blocking.
membrane fouling and flux decline [51]. Huang et al. [82] reported Besides, microbial community composition is effective on foul-
that longer SRTs (from 30 to infinite days) produced higher pro- ing. Gao et al. [46] found differences in community composition
tein/carbohydrate (P/C) ratio in EPS and lower P/C ratio in SMP, between the cake layer and biomass suspension for a membrane
which resulted in serious fouling. However, Herrera-Robledo coupled UASB reactor. They detected a bacterium within phyloge-
et al. [59] investigated the effect of SRT for both short and long- netic division OP11 at higher abundance in the cake layer com-
term operations for the system that used UF membrane as a polish- pared to the suspension. Moreover, some bacteria such as
ing step after a UASB reactor. It was found that fouling rate and Bacteroidetes were not found in the fouling layer although they ex-
effluent quality were not dependent on SRT. Their observations isted in the suspension. These results may indicate that some spe-
were based on trials for SRT of 60 and 100 days in short term oper- cies play a direct role in fouling, e.g. by attaching to the membrane
ation. Sudden changes in TMP and flux were observed for both surface, while others, including some that likely play a major role
SRTs. During long term operation (500 h), they observed that sud- in the metabolism of influent organics, play a less important or
den increases in TMP and decreases in flux occurred in shorter fil- indirect role. When this hypothesis is true it means that cells are
tration period (e.g. 140 h) with SRT of 60 days than with SRT of selectively incorporated within the fouling layer. Then, isolation
100 days (e.g. 175 h). This leads to the assumption that a more ri- and characterization of representatives of these species may pro-
gid and strong fouling layer structure was developed in the system vide useful information for biofouling control.
having long SRTs.

5.2.7. HRT 5.4. Addition of flux enhancers


Variations in HRT may change MBR fouling propensity. A few
researchers have reported the effect of HRT in membrane coupled The interest in flux enhancers that can act through a number of
sludge bed reactor types treating municipal wastewaters. Among different phenomena such as adsorption of SMP, coagulation,
them, An et al. [16] reported that a decrease in HRT from 10 h to crosslinking between flocs and SMP has greatly increased [87].
5.5 h resulted in a decrease in solids removal efficiency of the bio- Various additives such as activated carbon, polyelectrolytes, coag-
reactor. However, owing to the membrane separation, the reactor ulants and flocculants can be used to improve the flux and to re-
performance was quite stable. Besides, Lew et al. [48] observed duce fouling in MBRs [25,45].
that membrane fouling was positively correlated to the particulate Wu et al. [45] investigated poly-aluminum chloride as a flux en-
matter concentration reaching the membrane. hancer and found that addition of 10 mg/L poly-aluminum chloride
decreased fouling significantly in comparison to other tested
5.3. Sludge characteristics adsorbents/coagulants including PAC, zeolite, and polyamide. In
the study of Hu and Stuckey [25], the effects of PAC and GAC addi-
Currently EPS, both bound and soluble, is often mentioned as tion on TMP and flux were investigated in an AnMBR. In terms of
the sludge factor of prime importance in relation to membrane both TMP values and variations, better performances were
fouling. Soluble EPS is often also referred to as SMP [96]. Mem- achieved with activated carbon that constantly scoured deposited
brane inner pore accumulation and sorption of EPS and SMP favor particles from the membrane surface. Besides, a shift to a relatively
biomass attachment and cake layer formation, possibly leading to higher range in particle size distribution was observed in an
severe fouling [26,60]. Operational parameters such as SRT, OLR, AnMBR with activated carbon addition. On the other hand, particle
temperature, pH and shear rate are the most important factors size distribution shifted to a lower size range in the AnMBR with-
influencing both the concentration and composition of SMP and out activated carbon addition, which probably led to pore clogging.
EPS. Maintaining stable TMP and reducing fouling are more pronounced
EPS excreted from the microbial cells was considered to have a with PAC than with GAC due to the higher surface area of PAC.
significant effect on the fouling due to both an increase in viscosity Moreover, rigid PAC particles may also make the cake layer more
of the mixed liquor and an increase in the filtration resistance [98]. porous since they are larger than the bioflocs. Besides, Vyrides
Chu et al. [49] measured the amount of EPS from both granules in and Stuckey [39] observed a reduction in biofilm (gel layer) resis-
an AnMBR and sludge on the membrane surface and claimed that tance and thus, TMP reduction after the addition of PAC. However,
EPS affected the cake resistance by filling the void spaces between there appears to be an optimum dose for PAC addition. Extensive
the particles in the cake layer resulting in a drastic reduction in the addition can decrease the flux due to increased viscosity of the
flux. Viscosity of the liquor in the anaerobic reactor, which was sludge [86]. Akram and Stuckey [86] performed flux experiments
equal to the water viscosity, did not change with operating time. at a constant TMP and observed a significant flux improvement
Apparently, the impact of EPS is only on filtration resistance and from 2 L/m2 h to 9 L/m2 h with PAC addition of 1.67 g/L due to
not on liquid viscosity. An et al. [43] observed that EPS extracted the adsorption of fine colloids and dissolved organics, and the for-
from the cake layer consisted of mainly protein-like and humic mation of a thin cake layer on the membrane surface. However,
acid-like substances. Moreover, Gao et al. [46] found that EPS flux decreased with the addition of 3.4 g/L PAC as a result of the
mainly consisted of proteins and was the main reason of fouling viscosity increase. Due to the significant effects of additives on
in AnMBRs treating municipal wastewater. An et al. [43] reported mass transfer properties and biochemical environment and con-
that the support layer (non-woven fabric) surface was covered cerns related to cost effectiveness, the optimum dosage of addi-
with a rough and dense layer consisting of mainly protein, clay tives should be determined above which no further or even
materials and inorganic elements such as Mg, Al, Ca, Si, and Fe. adverse impacts can occur [87]. Most of the studies about the effect
SMP was grouped into two predominant fractions including of flux enhancers were done in short term experiments so far.
high and low molecular weight SMP in Herrera-Robledo et al.’s Therefore, the feasibility of continuous addition of these chemicals
100 H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104

during long term operation of AnMBRs treating municipal waste- fouling during long term operation can decrease the membrane life-
water still needs to be assessed. time in AnMBR applications. Kang et al. [88] identified struvite as
the most important inorganic foulant especially for inorganic mem-
branes. This would imply that inorganic fouling should not be
6. Cleaning methods underestimated in AnMBRs. However, despite the fact that there
are many investigations aimed at understanding the fouling mech-
The level and degree of membrane fouling depends on many anisms in membrane systems, the research on chemical cleaning is
factors such as membrane operation, reactor type, membrane con- very limited to either qualitative measurements, such as character-
figuration, substrate type and sludge characteristics. The cures and ization of membrane foulants and their cleaning removal efficiency,
cleaning methods can be various depending on the nature of foul- or permeability recovery observed after cleaning [99]. Thus far,
ing. Membrane cleaning can either be done physically or chemical cleaning is neither fully understood nor given the required
chemically. importance, which is critical for the development of better cleaning
Physical cleaning is closely related to membrane operation such agents and protocols, i.e. cleaning conditions, sequence and method
as regular backwash, relaxation or short term increase in shear rate [99]. More research should be conducted on membrane cleaning in
to remove the cake layer accumulated on the membrane surface. In order to fully understand the interaction between chemicals, fou-
addition, membranes can also be physically removed from the lants and membranes. This would definitely help to develop better
membrane tank to be cleaned ex situ, e.g. by applying water jets. cleaning practices and procedures for AnMBRs.
Cake layer formation on the membrane surface was found to play
the major role in the increase of membrane resistance and de-
crease of flux in AnMBRs [28]. As a matter of fact, Martinez-Sosa 7. Economic feasibility of AnMBRs for municipal wastewater
et al. [18] reported that the efficiency of physical cleaning in an treatment
AnMBR was close to 100% which indicated that irreversible fouling
was not notable or even did not exist. Economic efficiency is a key decisive criterion for the selection
In most literature, cleaning is generally understood as ‘cleaning of a process among competing technologies. High membrane sur-
in place’ (CIP), a chemical cleaning procedure done with alkali, oxi- face areas are required for the treatment of municipal wastewater
dants or acid cleaning agents. The CIP efficiency depends on many since influent flow rates are generally high. Therefore, AnMBRs are
factors, such as foulant type, substrate type, membrane material, particularly of interest if the (agricultural) use of the treated waste-
cleaning procedure, i.e. type of chemical, chemical concentration, water is considered. Within this concept, a feasibility study should
soaking/flushing duration, temperature, and frequency. be performed based on the energy consumption of pumps and ex-
Generally, an alkali cleaning solution such as NaOH and oxi- tra costs of additional membrane system devices and cleaning
dants such as H2O2 and NaOCl are effective in removing organic agents [15]. However, limited information is available in the liter-
foulants such as organic matter with carboxylic and phenolic ature about the economic efficiency of AnMBRs for municipal
groups, proteins and polysaccharides, whereas acid solutions wastewater treatment.
(HCl, H2SO4, citric acid) have been extensively used to remove inor- The reduced flux is known as the main factor determining the
ganic foulants such as metal hydroxides and divalent cations economic feasibility of membrane processes [103]. This unavoid-
[3,99]. Investigating municipal wastewater, Chu et al. [49] applied able disadvantage of AnMBR technology is associated with an in-
chemical cleaning for permeability recovery and compared two crease in operational costs, which arises from the requirement of
cleaning agents including only NaOCl and the combination of NaO- higher suction pressure, more intensive biogas recycling, larger
Cl and H2SO4 in terms of permeability recovery. No significant dif- membrane surface area and more frequent membrane cleaning
ference was observed between two washing methods. Chemical and replacement [59,96].
cleaning with NaOCl and backwashing methods were insufficient Lin et al. [23] assessed the economic feasibility of a submerged
to remove membrane biofouling in a membrane coupled UASB AnMBR system for municipal wastewater treatment based on over-
reactor [100]. Especially methanogenic Archaea remained undis- all costs. Overall costs are represented by the sum of capital costs
turbed by the chemical cleaning. Instead of these conventional including the costs of membranes, tanks and plant equipment and
cleaning methods, some advanced methods including nitric oxide operational costs which mainly comprise the costs of power,
cleaning, enzymatic disruption of exopolymers, bacteriophages, sludge disposal and chemicals. It was reported that membrane
etc. were proposed as effective cleaning techniques [46,100]. costs account for the largest fraction (72%) followed by the costs
Moreover, membrane material characteristics play a critical role of tank construction and screens among capital costs. Since mem-
on the application of different chemicals for cleaning, i.e. PP mem- brane costs are linearly correlated to the applicable flux, the ob-
branes are not chlorine tolerant or PVDF membranes cannot resist served low fluxes remain the obstacle for the potential
high pHs over 11 [99]. application of submerged AnMBRs in municipal wastewater treat-
The latest experience gained from aerobic MBRs treating muni- ment. For instance, similar to aerobic MBRs, coarse screening fol-
cipal wastewater suggests that frequent maintenance cleaning lowed by a fine screen should be considered in full scale systems
(weekly or monthly) at mild chemical concentrations can prevent in order to protect the membranes from damage and maximize
permeability loss during long term operation. That is, long term membrane life [23]. Gas scouring energy represents the most sig-
operation without any chemical cleaning results in residual mem- nificant operational cost. Operational costs for aerobic MBRs were
brane fouling that is difficult to remove with chemicals [101,102]. found three times higher than those for AnMBRs due to the in-
Moreover, frequent cleaning with dilute solutions consumes 30% creased blower energy and sludge disposal costs. Moreover, the
less reagents than infrequent cleaning that is applied i.e. quarterly operational costs for the AnMBRs can be partly offset by the use
or biennially using high-strength reagents [102]. of produced methane as an energy source [3]. Martin et al. [14] also
One of the greatest concerns about using chemicals for mem- reported that energy requirement associated with fouling control
brane cleaning is the effect of cleaning agents on membrane life- in AnMBRs was 2–3 times lower in comparison to the energy de-
time and integrity. Ayala et al. [102] suggested that a membrane mands of aerobic MBRs. However, due to the lower fluxes reported
lifetime of 6–7 years can be easily sustained in aerobic MBRs with- in literature for AnMBRs, the capital costs associated with mem-
out a significant loss of permeability and integrity if regular chem- branes might be higher compared to aerobic MBRs. They reported
ical cleaning is practiced. Inorganic fouling that causes irreversible a wide variation in energy demand (0.03–3.57 kW h/m3) in
H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104 101

submerged AnMBRs. Achilli et al. [40] compared the operational wastewater treatment by MBR systems [104–106]. In aerobic
costs of an aerobic MBR and AnMBR treating municipal wastewater MBRs, phenolic compounds, phthalates and estrogens can be more
and found that the operational costs of the AnMBR were lower effectively removed in comparison to conventional activated
than that of the aerobic MBR due to excess sludge management sludge systems through biodegradation, adsorption and membrane
in the aerobic MBR. However, the AnMBR system required a longer rejection mechanisms [104]. However, there exists very little infor-
acclimation time for stable operation than the aerobic MBR. Lin mation about their fate and biodegradation in AnMBRs [38]. Obvi-
et al. [23] also performed a sensitivity analysis including the effect ously, more research should be conducted on the fate of these
of variations in several aspects such as HRT, flux, membrane price, priority pollutants in AnMBR systems.
flow, membrane lifetime, interest and specific gas demand per unit Salinity can be another problem for the treatment of municipal
of membrane, and reported that influent flow exerted the largest wastewater, especially for coastal residential areas with improper
impact on the total life cycle costs since it determined the capacity infrastructure which allows the infiltration of sea water into sewer
and footprint of the system. Besides, costs are very sensitive to systems. Vyrides and Stuckey [39] examined the performance of a
changes in the applicable flux, membrane price and membrane submerged AnMBR treating saline municipal wastewater with high
lifetime followed by the moderate effect of interest. In contrast, fluctuations in salinity up to 35 g NaCl/L. They reported 99% re-
HRT and specific gas demand per unit of membrane were found moval of DOC at 35 g NaCl/L, however the removal efficiency inside
to influence the costs to a lesser extent. With the rapid develop- the reactor was very low (40–60% DOC). Their results indicated
ment and implementation of AnMBR technology especially in that the retention of SMPs and colloidal COD in the reactor was
full-scale systems, more research on economic analysis is required. due to membrane rejection. But in this situation more attention
should be given to fouling control in order to have a feasible treat-
ment technology.
8. Problems encountered and future perspectives When agricultural use of the treated effluent is not considered,
a nutrient removal step is generally required to comply with dis-
Upgrading of existing anaerobic treatment processes for muni- charge standards. Many studies report the effluent nutrient con-
cipal wastewater with membranes can be of vital importance, centration in AnMBRs treating municipal wastewater. Lin et al.
especially when high effluent quality and/or use of treated efflu- [23] did not observe any removal of nitrogen or total phosphorus
ents are considered. AnMBR effluents are pathogen free, which in an AnMBR treating municipal wastewater as expected. Herre-
makes them suitable for agricultural use [19,20]. However, the ra-Robledo et al. [60] also did not observe any decrease in ammo-
wide application of the AnMBRs in domestic utilities, especially nia concentration due to filtration. Interestingly, Kocadagistan and
in full-scale systems, has not yet become a reality, which is partly Topcu [15] observed phosphorus removal up to 81% in an AnMBR
because of system novelty and reluctance owing to membrane treating municipal wastewater by membrane retention. Similar re-
fouling problems [49]. Therefore, AnMBR systems will likely bene- sults with regard to phosphorus removal together with calcium,
fit from the development of efficient technologies to prevent magnesium and iron were reported by Herrera-Robledo et al.
fouling. [60]. Moreover, Saddoud et al. [51] reported high nitrogen and
Inorganic fouling by the precipitation of struvite (MgNH4PO4- phosphorus removal, such as 60% and 30% respectively, in an
6H2O), K2NH4PO4 and/or CaCO3 may be one of the major concerns AnMBR which may not be explained solely by the uptake of these
in fouling due to the release of ammonia and phosphate from or- macronutrients by biomass growth. Removal of these elements
ganic nitrogen and phosphorus during AD and pH increases as a re- with low molecular sizes in comparison to the membrane nominal
sult of changes in carbon dioxide partial pressure and alkalinity cut-off may be attributed to their sorption by the biofouling layer
generation in AnMBRs [3]. Salazar-Pelaez et al. [61] estimated that or even chemical precipitation. These contradictory results are
struvite would be undersaturated in municipal wastewaters with mainly due to the differences in membrane rejection capabilities
2 +
lower concentrations of NHþ 4 ; PO4 and Mg compared to industrial of the systems in different studies.
wastewaters and struvite precipitation would unlikely occur. How- More research needs to be directed towards the applicability of
ever, not only the concentration of these ions but also the mem- AnMBR to low-temperature municipal wastewaters. A significant
brane properties can play a significant role in struvite reduction in the hydrolysis rate of solids is typical at ambient tem-
precipitation [88]. Therefore, this phenomenon which may cause peratures due to the low activity of anaerobic microorganisms
irreversible fouling should be further investigated with long term [5,26]. Methane loss is another important issue of concern espe-
studies in AnMBRs treating municipal wastewaters. cially at low temperature processes since methane solubility in
Other major concerns about using treated municipal wastewa- the liquid phase increases with decreasing temperature. Gimenez
ter in agriculture are related with the removal of toxicity and endo- et al. [42] proposed biogas-assisted mixing as a limitation for
crine disrupting chemicals. Industrial discharges to municipal super-saturation and a guarantee for a minimum concentration
sewer systems can cause serious problems such as toxicity and or- of dissolved methane in the effluent of AnMBR systems.
ganic shock loads in the end-of-pipe wastewater treatment plants. Alternative membrane materials, reactor types, and membrane
Saddoud et al. [20] using an AnMBR equipped with a cross-flow UF integration possibilities and configurations for AnMBR technology
module investigated the treatability of municipal wastewater com- in municipal wastewater treatment schemes are of interest to fur-
prising industrial discharges containing toxic substances. The ther develop. Dynamic membrane technology that focuses on the
AnMBR process was found to be inefficient, in terms of unstable use of meshes or fabrics as a support material instead of real mem-
biogas production rate and composition, due to the high fluctua- branes is gaining interest in the AnMBR applications for municipal
tions in the industrial toxicants. Besides, Ellouze et al. [19] ob- wastewater treatment. Application of dynamic membrane systems
served a residual toxicity in wastewaters treated with AnMBRs will significantly reduce capital costs associated with the purchase
due to the toxic soluble compounds from industrial discharges into and renewal of membranes [26,107]. So far, there have been several
the sewer, which passed through the membrane. However, the attempts to utilize dynamic membrane filtration in AnMBR systems
permeate obtained from the AnMBR was found to be significantly and the results in terms of removal efficiency were very promising
less toxic than the effluent of conventional treatment processes, and comparable to conventional membranes [26,38,43,47]. How-
such as aerated lagoon and activated sludge, based on micro-toxic- ever, more research should be conducted to understand the forma-
ity and phyto-toxicity analysis. Various studies address the re- tion mechanisms of dynamic membrane (cake) layer and to
moval of endocrine disrupting chemicals in municipal effectively control it for beneficial use of filtration.
102 H. Ozgun et al. / Separation and Purification Technology 118 (2013) 89–104

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AnMBR permeate may be used in agriculture or the nutrients in [15] E. Kocadagistan, N. Topcu, Treatment investigation of the Erzurum City
the permeate may be recovered in order to get full benefit from the municipal wastewaters with anaerobic membrane bioreactors, Desalination
216 (2007) 367–376.
advantages offered by this technology. Combination of membranes
[16] Y.Y. An, F.L. Yang, B. Bucciali, F.S. Wong, Municipal wastewater treatment
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