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Journal of Environmental Science and Health, Part A: Toxic/Hazardous Substances and Environmental Engineering
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Wastewater treatment in a submerged anaerobic membrane bioreactor

Stefania Casu , Nedda A. Crispino , Roberto Farina , Davide Mattioli , Marco Ferraris & Alessandro Spagni
a a a a a a a

ENEA (Italian National Agency for New Technologies, Energy and Sustainable Economic Development), Water Resource Management Section, Bologna, Italy Published online: 13 Jan 2012.

To cite this article: Stefania Casu , Nedda A. Crispino , Roberto Farina , Davide Mattioli , Marco Ferraris & Alessandro Spagni (2012): Wastewater treatment in a submerged anaerobic membrane bioreactor, Journal of Environmental Science and Health, Part A: Toxic/Hazardous Substances and Environmental Engineering, 47:2, 204-209 To link to this article: http://dx.doi.org/10.1080/10934529.2012.640562

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Journal of Environmental Science and Health, Part A (2012) 47, 204209 Copyright C Taylor & Francis Group, LLC ISSN: 1093-4529 (Print); 1532-4117 (Online) DOI: 10.1080/10934529.2012.640562

Wastewater treatment in a submerged anaerobic membrane bioreactor

STEFANIA CASU, NEDDA A. CRISPINO, ROBERTO FARINA, DAVIDE MATTIOLI, MARCO FERRARIS and ALESSANDRO SPAGNI
ENEA (Italian National Agency for New Technologies, Energy and Sustainable Economic Development), Water Resource Management Section, Bologna, Italy

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Although most membrane bioreactors are used under aerobic conditions, over the last few years there has been increased interest in their application for anaerobic processes. This paper presents the results obtained when a bench-scale submerged anaerobic membrane bioreactor was used for the treatment of wastewaters generated in the agro-food industry. The reactor was fed with synthetic wastewater consisting of cheese whey and sucrose, and volumetric organic loading rates (OLRs) ranging from 1.5 to 13 kgCOD/(m3 d) were applied. Under the operating conditions studied, the maximum applicable OLR was between 6 and 10 gCOD/(g L), which fell within the ranges of the high-rate anaerobic wastewater treatment systems, while high concentrations of volatile fatty acids were produced at higher OLR rates. With an OLR of 1.510 gCOD/(g L), the reactor showed 94% COD removal, whereas this value dropped to 33% with the highest applied OLR of 13 gCOD/(g L). The study therefore conrms that membrane bioreactors can be used for anaerobic wastewater treatment. Keywords: Membrane bioreactor, anaerobic digestion, wastewater treatment, biogas.

Introduction
Over the last decade, membrane bioreactors (MBRs) have been successfully used for treating municipal and industrial wastewater. Two different MBR process congurations have been applied: external, where the membrane modules are situated outside the bioreactor, and submerged where the membranes are directly immersed in the reactor tank. Most submerged MBRs are applied under aerobic conditions where aeration is also used to create the cross-ow along the membrane to reduce fouling.[13] Nevertheless, anaerobic treatments provide several advantages as compared to aerobic ones, mainly due to the energy balance achieved by biogas production and to the lower amount of sludge produced. The efcacy of every biological wastewater treatment process is related to decoupling of the solids retention time (SRT) from the hydraulic retention time (HRT) so as to obtain high biomass concentrations and, thus, high treatment rates. Most of the high-rate anaerobic systems use biolm or granular sludge to achieve a high concentration

Address correspondence to Alessandro Spagni, ENEA, Environment Department, via M.M. Sole, 4 40129, Bologna, Italy; Email: alessandro.spagni@enea.it. Received April 13, 2011.

of biomass. When biolm or granulation cannot be easily achieved (e.g., due to a high concentration of suspended solids in the wastewater), membrane separation could represent an alternative as it allows a high concentration of biomass to be obtained in the reactor, thereby maintaining high treatment rates.[4,5] To reduce caking on the membranes and the resulting membrane fouling in submerged anaerobic MBRs (SAMBRs), the produced biogas can be recirculated and used for scouring the membrane instead of the air bubbling of submerged aerobic MBRs.[4,5] Anaerobic MBRs (AMBRs) have recently received a great deal of attention from researchers.[6] Most of the AMBRs in wastewater treatments have used the external conguration[4,7] although over the last few years there has been increased research into SAMBRs.[825] Because the energy requirement for submerged MBRs is usually much lower than for the side stream ones (at least for aerobic systems),[12] application of SAMBRs could represent a further improvement in the energy balance of the wastewater treatment plant. Moreover, since the anaerobic processes are related to strict interactions among several microbial populations, the shear stress on the biomass caused by pumps in the side stream conguration has been envisaged as an important cause of reduced biomass activity and membrane permeability.[26,27] The majority of the studies on SAMBRs have dealt with membrane fouling

Wastewater treatment in membrane bioreactor

and mainly with the causes and the reduction/control of the fouling processes.[1215, 28] Due to the variability of the applicable anaerobic conditions (psychrophilic, mesophilic or thermophilic), of the membranes available on the market as the conguration (external or immersed) or the wastewater that can be potentially treated, the knowledge about membrane-assisted anaerobic processes still remains limited. In this study, a laboratory-scale SAMBR was used with the aim of identifying the main operating conditions for membrane-assisted anaerobic wastewater treatment. The lterability characteristics of the proposed system were previously investigated,[28] while this study assesses the treatment efciency in terms of COD removal and biogas production.
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D: 24 90 10 cm), a working volume of approximately 11 L and was operated at 351 C in a thermostatic room for almost 250 days. The volume of the headspace was approx. 10 L to prevent the foaming problems that can be caused by biogas recirculation. A at sheet membrane module (Kubota R , of mm 225 315 (W H) with a ltration area of 0.12 m2 and 0.4 m nominal pore size) immersed in the sludge was used. Sludge mixing and membrane scouring to control fouling were achieved by recirculating the biogas through a coarse diffuser situated just below the membrane module. The biogas ux was approximately 20 L/min (all the gas values given in this paper refer to standard conditions), which resulted in a supercial velocity of 56 m/h (calculated considering the transversal area of the reactor). Biogas was recirculated using a vacuum/compressor pump (KNF) and the gas ow was regulated with a variable area owmeter (Cole-Parmer International). Filtration was carried out by alternating 4 minutes of ltration and 1 minute of relaxation: no backwash was applied. The treated water was extracted from the membrane by applying a vacuum with a programmable piston pump (Cole-Parmer International). Trans membrane pressure (TMP) was measured with a digital gauge (Cole-Parmer International). No sludge was extracted for the rst 50 days (except for small samples so as to measure the solids). After this, due to a high increase in TMP[28], sludge was extracted to control the total suspended solids (TSS) and TMP. Thereafter, the solids retention time (SRT) was controlled at approximately 50 days, except between days 150 and 190, when the SRT was increased again (so as to increase the sludge concentration), resulting in a sludge age of approx. 600 d.

Materials and methods

Experimental setup The study was conducted using a laboratory-scale SAMBR (Fig. 1). The reactor has a total volume of 21.6 L (W H

Effluent

Gasmeter

Synthetic wastewater and inoculum

Flowmeter

Influent

Fig. 1. Schematic diagram of the laboratory scale SAMBR.

The SAMBR was fed for the rst 160 days with synthetic wastewater comprising dried cheese whey and sucrose (usually 1:1 as COD) as organic matter. After this, the feed was entirely formed by sucrose. A salt solution consisting of NH4 Cl (approx. 0.02 gN/gCOD), K2 HPO4 (approx. 0.01 gP/gCOD), NaHCO3 (approx. 0.5 g/gCOD), FeCl2 (0.35 mg Fe/L) and Na2 MoO4 (0.02 mgMo/L) was also fed into the reactor. The feed solution was prepared by continuously diluting concentrated solutions with tap water just before adding them to the reactor (note that membrane fouling inuenced the ows and, thus, the feed concentration). During the study, the feed concentration and the HRT were intentionally varied in order to evaluate both the ltration characteristics[28] and removal efciencies under different operating conditions. The plant was seeded with approximately 1 kg of wet granular sludge taken from a full-scale upow anaerobic sludge blanket reactor treating agro-industrial wastewater. The shear stress on the membrane caused by biogas recirculation gradually crushed

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the granules, which completely disappeared after approximately 3040 days of experimentation. Analysis COD, TSS and volatile suspended solids (VSS) were measured according to Standard Methods.[29] The volatile fatty acids (VFAs: acetic, propionic, n-butyric, i-butyric, valeric, caproic and heptanoic) and the biogas composition were measured by gas chromatographic techniques as described elsewhere.[30] Sucrose was measured according to Dubois et al.[31] Biogas production was measured using a homemade wet-tip gas-meter. Sample ltration was performed using Whatman GF/C lters.
HRT (d) 140 120 100 80 60 40 20 0 CODin CODout

Casu et al.
(a)

(b)

30 25 20 15 10 5 0 COD (g/L)
250

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Results and discussion

Although the anaerobic sludge lterability trend in the MBR has been extensively described elsewhere,[28] we would like to stress that the low lterability observed resulted in severe fouling events which caused the operating conditions to frequently change (especially as the experiments were conducted) due to changes in the applicable uxes on the membrane and thus, in the HRT. The severe fouling occurrences[28] actually resulted in several cases of uncontrolled HRT, which caused even higher variable organic loading rates (OLRs), especially during the second part of the study. As a result, volumetric organic loading of the reactor ranged from 1.5 to 13 kg COD/(m3 d), with the exception of 2 periods where ltration was turned off for maintenance and holidays. Figure 2 illustrates the applied HRTs, the inuent COD concentration (with the efuent COD) and the resulting OLRs. During the rst 50 days of experimentation, the mixed liquor TSS (MLTSS) increased continuously from 5.5 to 20.4 g/L since no sludge was drawn off. After this, owing to the TMP buildup,[28] the ltration was switched off (biogas recirculation remained on; Fig. 2) and some sludge (approximately 56 L) was extracted to lower the TSS concentration to under 10 g/L (Fig. 3). After 5 days of gas scouring on the membrane without ltration, the TMP dropped to values that allowed the ltration process to be restarted. The plant was then operated at an approximately constant OLR of 1.61.7 gCOD/(L d) for another 10 days until the holidays (2 weeks), when it was turned off completely. After day 85, the ORL was gradually increased (Fig. 2c) from 1.6 to 6 gCOD/(L d) over a period of about 70 days: for approximately 50 days, the solids concentration remained almost stable at 7.71.2 (mean standard deviation of n = 13 samples) and 6.40.9 g/L for TSS and VSS, respectively, and then the values increased to 21.0 and 17.9 g/L for TSS and VSS, respectively. The low TSS values (Fig. 3) measured after approximately 150 days of experimentation were due to the sludge being removed from the reactor in order to assess sludge l-

16 14 12 10 8 6 4 2 0 0 50 100 150 Time (d) 200

OLR [gCOD/(L*d)]

(c)

250

Fig. 2. Hydraulic retention time (HRT) (a), inuent (CODin) and efuent COD (CODout) (b) and resulting organic loading rate (OLR) (c).

terability at a low TSS concentration. The extracted sludge was put back into the reactor immediately after the test. From day 161 to the end of the study, the feed was composed by sucrose only. The OLR was increased to the maximum values of approximately 13 kgCOD/(m3 d), maintaining low uxes on the membrane.[28] Although it was not possible to apply a constant load (Fig. 2c), the increased load and SRT caused an increase of the solids concentration
60

Suspended Solids (g/L)

50 40 30 20 10 0 0 50 100 150 200

Time (d)
Fig. 3. MLTSS and MLVSS in the reactor during the experimental campaign.

Wastewater treatment in membrane bioreactor

1.0
12

207

Volatile fatty acids (g/L)

y = -0.0044x + 0.8703
0.9

VSS/TSS

R = 0.4923 P < 10-8

10 8 6 4 2 0

Acetic Propionic n-butyric

0.8

Giorno vs SST (g/L)

0.7

0.6 0 10 20 30 40 50 60

50

100

150

200

250

TSS (g/L)

Time (d)

Fig. 4. Linear regression analysis of the VSS/TSS ratios versus TSS concentration.

Fig. 6. Concentrations of the main volatile fatty acids measured.

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in the reactor (Fig. 3), which reached the maximum value measured during the experiment, i.e., 53 and 40 g/L for TSS and VSS, respectively. Again, the membrane uxes had to be decreased due to the increased TMP, thus affecting the applied OLR. Although the extremely varied operating conditions made it difcult to assess the sludge yield, it was roughly estimated[32] as being between 0.03 and 0.06 gVSS/g COD removed (observed growth yield), depending on the operating conditions, which fell within the typical values for anaerobic processes.[33] As already observed for aerobic MBR by other authors,[34] the increased solids concentration tended to cause inert materials to build up inside the reactor, as demonstrated by the way the VSS/TSS ratios decreased as the solids concentration in the reactor increased (Fig. 4). Unlike other high-rate anaerobic systems where highefuent suspended solids concentrations are usually observed,[35] the TSS in the SAMBR efuent were completely absent due to membrane cutoff (0.4 m). During the rst 150 days of the study, the reactor was fed with
120 100 80

3.0 g/L constant-COD synthetic wastewater. The lab-scale SAMBR showed very good COD removal (Fig. 5) even with variable OLR (Fig. 2c) due to variable HRT (Fig. 2a). Efuent COD concentration and COD removal were 200259 mg/L (n = 30; median = 96 mg/L) and 948% (n = 30; median = 97), respectively. The COD removal measured in this study was in keeping with the ndings of other studies.[22] Complete sludge retention by the membrane greatly affected the efuent COD, to the extent that it consisted of soluble organics only. When the increased loading rate was applied after day 150, a signicant decrease in COD removal was observed, as it dropped to the minimum value of 33%. The highest applied OLR of 13 and 11 gCOD/(L d) therefore seemed to overload the system. When the OLR dropped to 56 gCOD/L, the reactor tended to restabilise even though rather slowly. The drop in COD removal was caused by the VFAs that built up in the mixed liquor (Fig. 6). Although propionic acid was the most abundant soluble organic when overloading began, after this the acetic acid rapidly increased until it reached the highest concentration of 10.03 g/L.
7.5

COD removal (%)

7.0

pH
60 40 20 0 50 100 150 200 250

6.5

6.0

5.5 0 50 100 150 200 250

Time (d)

Time (d)

Fig. 5. COD removal efciency during the study.

Fig. 7. pH trend measured during the study.

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Casu et al.
lead to an increase in the concentration of biomass and, thus, the applicable OLR.

Biogas production (L/d)

50 40 30 20 10 0 0 50 100 150 200 250

Acknowledgments
This study was partially supported by the European Union within the framework of the AquaFit4use project (ENV.2007.3.1.1.1211534).

References
[1] Stephenson, T.; Brindle, K.; Judd, S.; Jefferson, B. Membrane bioreactor for wastewater treatment; IWA Publishing: London, UK, 2000. [2] Judd, S. The MBR book; Elsevier: Amsterdam, The Netherlands, 2006. [3] Van der Roest, H.F.; Lawrence, D.P.; Van Bentem, A.G.N. Membrane bioreactors for municipal wastewater treatment, STOWA Report; IWA Publishing: London, UK, 2002. [4] Liao, B.-Q.; Kraemer, J.T.; Bagley, D.M. Anaerobic membrane bioreactors: applications and research directions. Crit. Rev. Env. Sci. Tec. 2006, 36(6), 489530. [5] Van Lier, J.B.; Tilche, A.; Ahring, B.K.; Macarie, H.; Moletta, R.; Dohanyos, M.; Hulshoff Pol, L.W.; Lens, P.; Verstraete, W. New perspectives in anaerobic digestion, Water Sci. Technol. 2001, 43(1), 118. [6] Le-Clech, P. Membrane bioreactors and their uses in wastewater treatments. Appl. Microbiol. Biotechnol. 2010, 88(6), 12531260. [7] Ho, J.; Sung, S. Anaerobic membrane bioreactor treatment of synthetic municipal wastewater at ambient temperature. Water Environ. Res. 2009, 81(9), 922928. [8] Hu, A.Y.; Stuckey D.C. Treatment of dilute wastewaters using a novel submerged anaerobic membrane bioreactor. J. Environ. Eng.ASCE, 2006, 132(2), 190198. [9] Trzcinski, A.P.; Stuckey, D.C. Anaerobic digestion of the organic fraction of municipal solid waste in a two-stage membrane process. Water Sci. Technol. 2009, 60(8), 19651978. [10] Trzcinski, A.P.; Stuckey, D.C. Treatment of municipal solid waste leachate using a submerged anaerobic membrane bioreactor at mesophilic and psychrophilic temperature: analysis of recalcitrants in the permeate using GC-MS. Water Res. 2010, 44(3), 671680. [11] Jeison, D.; Van Lier, J.B. Anaerobic wastewater treatment and membrane ltration. Water Sci. Technol. 2008, 57(4), 527532. [12] Jeison, D.; Van Lier, J.B. Bio-layer management in anaerobic membrane bioreactors for wastewater treatment, Water Sci. Technol. 2006, 54(2), 8186. [13] Jeison, D.; Van Lier, J.B. Thermophilic treatment of acidied and partially acidied wastewater using an anaerobic submerged MBR: factors affecting long-term operational ux, Water Res. 2007, 41(17), 38683879. [14] Jeison, D.; Van Lier, J.B. Cake layer formation in anaerobic submerged membrane bioreactors (AnSMBR) for wastewater treatment, J. Membrane Sci. 2006, 284(12) 227236. [15] Jeison, D.; Van Lier, J.B; Cake formation and consolidation: main factors governing the applicable ux in anaerobic submerged membrane bioreactors (AnSMBR) treating acidied wastewaters, Sep. Purif. Technol. 2007, 56(1), 7178. [16] Jeison, D.; van Lier, J.B.; Feasibility of thermophilic anaerobic submerged membrane bioreactors (AnSMBR) for wastewater treatment. Desalination 2008, 231(13), 227235. [17] Kanai, M.; Ferre, V.; Wakahara, S.; Yamamoto, T.; Moro, M. A novel combination of methane fermentation and MBR Kubota submerged anaerobic membrane bioreactor process. Desalination 2010, 250(3), 964967.

Time (d)

Fig. 8. Biogas production trend during the study.

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Along with acetic acid, n-butyric acid also gradually increased to the maximum value of 3.15 g/L. With the drop in applied OLR after experimental day 160, all the VFAs gradually decreased to approximately the values measured at the beginning of the study. The other VFAs measured always presented concentrations that were below 300 mg/L. The sugars concentration in the reactor efuent was always below the detection limit of the instrument, conrming the methanogenic activity of the acetoclastic bacteria as the limiting kinetic process in biogas production,[33] at least for the simple sugar (sucrose) used in this study. The increase in OLR was also shown by the lower pH in the mixed liquor due to VFA build-up (Fig. 7); in fact, the higher the OLR the lower the pH, conrming yet again that the system approximated the overload with the highest applied OLR. Biogas production was also extremely variable due to the highly variable operating conditions applied (Fig. 8). Biogas production followed the applied OLR and COD removal in an almost proportional way, indicating that the system was sufciently robust to cope with the approaching overload. The biogas was also slightly variable as to composition, with the methane content ranging from 49 to 67% and carbon dioxide as the remaining fraction.

Conclusions
The study conrmed that membrane bioreactors can be used for anaerobic wastewater treatment. Under the studied operating conditions, the maximum applicable OLR was between 6 and 10 gCOD/(g L), which fell within the ranges of the high-rate anaerobic wastewater treatment systems (e.g., UASB) and other SAMBRs.[25] SAMBRs therefore seem to be an alternative system for anaerobic wastewater treatment when other high-rate systems cannot be applied. Due to the low lterability of the anaerobic sludge,[28] the maximum biomass concentration obtained in the system was 4050 gTSS/L. Improved lterability could therefore

Wastewater treatment in membrane bioreactor

[18] Van Zyl, P.J.; Wetzel, M.C.; Ekama, G.A.; Riedel, K.J. Design and start-up of a high rate anaerobic membrane bioreactor for the treatment of a low pH, high strength, dissolved organic waste water. Water Sci. Technol. 2008, 57(2), 291295. [19] Hall, E.R.; B erub e, P.R. Membrane bioreactors for anaerobic treatment of wastewaters: phase II; WERF report (Alexandria); IWA Publishing: London, UK, 2006. [20] Huang, Z.; Ong, S.L.; Ng, H.Y. Feasibility of submerged anaerobic membrane bioreactor (SAMBR) for treatment of low-strength wastewater. Water Sci. Technol. 2008, 58(10):19251931. [21] Gao, W.J.J.; Lin, H.J.; Leung, K.T.; Liao, B.Q. Inuence of elevated pH shocks on the performance of a submerged anaerobic membrane bioreactor. Process Biochem. 2010, 45(8), 12791287. [22] Huang, Z.; Ong, S.L.; Ng, H.Y. Submerged anaerobic membrane bioreactor for low-strength wastewater treatment: effect of HRT and SRT on treatment performance and membrane fouling. Water Res. 2011, 45(2), 705713. [23] Vyrides, I.; Santos, H.; Mingote, A.; Ray, M.J.; Stuckey D.C. Are solutes compatible with biological treatment of saline wastewater? Batch and continuous studies using submerged anaerobic membrane bioreactors (SAMBRs). Environ. Sci. Technol. 2010, 44(19), 74377442. [24] Xie, K.; Lin, H.J.; Mahendran, B.; Bagley, D.M.; Leung, K.T.; Liss, S.N.; Liao, B.Q. Performance and fouling characteristics of a submerged anaerobic membrane bioreactor for kraft evaporator condensate treatment. Environ. Technol. 2010, 31(5), 511 521. [25] Liao, B.Q.; Xie, K.; Lin, H.J.; Bertoldo, D. Treatment of kraft evaporator condensate using a thermophilic submerged anaerobic membrane bioreactor. Water Sci. Technol. 2010, 61(9), 21772183.

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[26] Ghyoot, W.R.; Verstraete, W. Coupling membrane ltration to anaereobic primary sludge digestion. Environ. Technol. 1997, 18, 569580. [27] Kim, J.S.; Lee, C.H.; Chang, I.S. Effect of pump shear on the performance of a crossow membrane bioreactor. Water Res. 2001, 35, 21372144. [28] Spagni, A.; Casu, S.; Crispino, N.A.; Farina, R.; Mattioli, D. Filterability in a submerged anaerobic membrane bioreactor. Desalination 2010, 250(2), 787792. [29] APHA, AWWA, WEF, Standard Methods for the Examination of Water and Wastewater, 21st ed., Washington, DC, 2005. [30] Spagni, A.; Casu, S.; Farina, R. Effect of the organic loading rate on biogas composition in continuous fermentative hydrogen production. J. Environ. Sci. Health A 2010, 45(12), 14751481. [31] Dubois, M.; K. Gilles, A.; Hamilton, J. K.; Rebers, P. A.; Smith, F. Colorimetric method for determination sugars and related substances. Anal. Chem. 1956, 28, 350356. [32] Henze M.; Harremoes, P.; Jansen, J.la.C.; Arvin E. Wastewater treatment: biological and chemical processes, 3rd edition; SpringerVerlag: Berlin, 2000; 430 pp. [33] Van Lier, J.B.; Mahmoud, N.; Zeeman, G. In Anaerobic wastewater treatment, in Biological wastewater treatment: principles, modelling and design; Henze, M.; Van Loosdrecht, M.C.M.; Ekama, G.A.; Brdjanovic, D., Eds.; IWA Publishing: London, UK, 2008; 415456. [34] Laera, G.; Pollice, A.; Saturno, D.; Giordano, C.; Lopez, A. Zero net growth in a membrane bioreactor with complete sludge retention. Water Res. 2005, 39(20), 52415249. [35] Tchobanoglous, G.; Burton, F.L.; Stensel, H.D. Wastewater engineering: treatment and reuse; Metcalf & Eddy Inc. McGraw-Hill Companies: New York, 2003; 1819 pp.

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