Development of an integrated membrane process for water reclamation

C.H. Lew*, J.Y. Hu*, L.F. Song*, L.Y. Lee*, S.L. Ong*, W.J. Ng* and H. Seah**
*Environmental Science and Engineering Programme, National University of Singapore, 10 Kent Ridge Crescent, Singapore 119260 (E-mail: cvehujy@nus.edu.sg) **Public Utilities Board, 40 Scotts Road, Singapore 228231 Abstract An integrated membrane process (IMP) comprising a membrane bioreactor (MBR) and a reverse osmosis (RO) process was developed for water reclamation. Wastewater was treated by an MBR operated at a sludge retention time (SRT) of 20 days and a hydraulic retention time (HRT) of 5.5 h. The IMP had an overall recovery efficiency of 80%. A unique feature of the IMP was the recycling of a fraction of RO concentrate back to the MBR. Experimental results revealed that a portion of the slow- and hard-to-degrade organic constituents in the recycle stream could be degraded by an acclimated biomass leading to an improved MBR treatment efficiency. Although recycling concentrated constituents could impose an inhibitory effect on the biomass and suppress their respiratory activities, results obtained suggested that operating MBR (in the novel IMP) at an F/M ratio below 0.03 g TOC/g VSS.day could yield an effluent quality comparable to that achievable without concentrate recycling. It is noted in this study that the novel IMP could achieve an average overall TOC removal efficiency of 88.94% and it consistently produced product water usable for high value reuse applications. Keywords Biomass acclimation; integrated membrane process; membrane bioreactor; reverse osmosis; slow- and hard-to-degrade compounds; water reclamation

Water Science & Technology Vol 51 No 6–7 pp 455–463 Q IWA Publishing 2005

Introduction

Economic development and global industrialization over the past decades have inevitably heightened the conflict between water demand and water supply. Consequently, water reclamation has increasingly been receiving attention and seriously explored and/or exploited in many parts of the world for augmenting freshwater supplies. In most cases, membrane technology has been employed and that more than one membrane processes are typically used in order to obtain the benefits associated with multiple barriers provided by such arrangement and to assure product water with high quality and purity. One such advanced reclamation technology is the coupling of an MBR with a downstream RO process whereby the MBR is used to serve as a pretreatment to the RO process. In this configuration, soluble microbial products (SMP) could potentially be an issue that may impede the performance of the integrated MBR-RO system (i.e. IMP). SMP are defined as the pool of organic compounds that are released into solution from substrate metabolism accompanied by biomass growth, and biomass decay (Duncan and David, 1999). SMP has been said to be inert in nature. It has been shown that the majority of soluble organic matters in effluents from biological treatment processes are actually SMP, and hence its presence could significantly affect the effluent quality. Similarly, in the treatment of industrial wastewater, the presence of inherent refractory organics can also significantly affect the quality of the final treated effluent. In view of this, it could be expected that the major constituents in the effluent of a biotreatment system treating mixed municipal and industrial wastewater would likely contain SMP and wastewater inherent refractory organic compounds.

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5.. carrying out concentrate recycling may facilitate: (i) degradation of any residual easily degradable organic matters present in the recycle stream.and hard-to-degrade organic compounds. causing plasmolysis and loss of cell activity. MBR could facilitate selective growth of specific microorganisms for the degradation of hardly degradable hazardous substances (Yamamoto.and hard-to-degrade organic compounds present in the RO concentrate stream produced from the IMP. 2001). organisms which in turn results in better removal of refractory organic matters (Co 1997). In this study. and (ii) degradation of a portion of the slow. Lew et al. membrane cleaning was . In view of the above.0 to 7.and hard-to-degrade organic compounds via concentrate recycling (which would otherwise be wasted via the RO bleed line in an IMP without recycling) will result in a less concentrated RO concentrate waste stream. This observation suggested that one could recycle a fraction of the RO concentrate back to the MBR operated at a long SRT and exploit the MBR for treating slow. This achievement can also help to reduce the adverse environmental effects due to concentrated waste disposal. In addition. 1996). If these desired aims could be achieved. Membrane filtered effluent was intermittently discharged at a constant flux by a suction pump..5 h and a SRT of 20 days.45 mm pore size.. 2000. SMP is noted to be biodegradable over time. In view of this. That is. High concentration of SMP in an MBR was reported to be inhibitory to the metabolic activity of the activated sludge (Huang et al. These concerns need to be adequately addressed in order for the proposed novel IMP to be technically feasible. it has been reported that operating MBR at a SRT greater than 20 days could allow the development of slow-growing microˆ te ´ et al. the objective of this research is to study the operating characteristics of using an IMP to reclaim high quality product water from mixed industrial and domestic wastewater. Methods 456 C. This is because MBR could allow the establishment of specialized microorganisms capable of removing slowly degradable components (Rosenberger et al. The need for a higher suction pressure to maintain a constant permeate flux gave an indirect indication of membrane fouling. Another concern is the deterioration of MBR effluent quality due to the concentrate recycling. The total ML volume in the bioreactor was 16. high levels of total dissolved solids (TDS) have been known to produce an osmotic pressure on cells. The MBR was operated at a constant HRT of 5.825 L of ML was wasted daily in order to maintain a desired SRT. For example. A review of literature revealed that an increase in the concentrations of non-reactive compounds in bioreactors at long SRT can lead to microbial inhibition or toxicity (Brindle and Stephenson. The schematic diagram of the novel IMP is shown in Figure 1.One of the potential advantages offered by the MBR is that it could allow the biodegradation of slow. although the kinetics of degradation may be much slower than simple substrates. Similarly. Shin and Kang.and hard-to-degrade organic compounds present in both the recycle stream and MBR Mixed Liquor (ML). SMP and wastewater inherent refractory organic compounds in the MBR ML. degradation of a portion of these slow. The ML dissolved oxygen (DO) level was always above 5 mg/L. It has been reported that SMP biodegradation occurred in MBRs after an acclimation period (Huang et al. due to potential elevated concentrations of TDS. pH in the bioreactor was maintained within a range of 7. Each intermittent suction cycle consisted of an 8 mins suction period followed by a 2 mins non-suction period. The MBR was operated with two submerged Kubota flat sheet microfiltration membranes of 0.5 L and 0. a primary concern in the operation of the novel IMP will be the inhibition and potential intoxication of microorganisms.. it will enhance MBR treatment efficiency and improve overall performance of the novel IMP. 2002).H. In addition. 2003). 2000).

A concentrate flow rate equal to 20% of the wastewater influent rate was internally recycled back to the MBR. Lew et al. the TDS and total organic carbon (TOC) concentrations of the RO feed were higher than the MBR effluent. RO concentrate and RO permeate. 457 .%) and sodium tripolyphosphate (2. as compared with the NH3-N and TDS concentrations. Chemical cleaning was carried out once every 3–4 months by immersing the membranes in sodium hypochlorite solution (0. Figure 1 Schematic flow diagram of the IMP system initiated once suction pressure exceeded 5. TOC. The experimentation period was divided into four phases. As bulk of the RO concentrate stream was recycled back to the effluent tank.C.84 wt. Phase 4 represented the stabilization and operation of the novel IMP at a SRT of 20 days for 147 days.H. This allowed the IMP to achieve an overall recovery efficiency of 80%.5 wt. Primary settled effluent was collected from the WWTP and the wastewater has a 60% industrial and 40% municipal wastewater composition. Phase 1 represented the seeding and start-up of the MBR for 114 days. MLSS. A single thin film GE Osmonics RO membrane element was used for the RO process. Shimadzu) were conducted for all the samples. Assessment of microbial viability was carried out based on the specific oxygen uptake rate (sOUR).5 wt. Ammonia nitrogen. the RO process was operated in a concentrate recirculation mode. the wastewater strength in terms of TOC was highly variable. chemical cleaning was initiated. The seed sludge and wastewater source for the four phases were collected from a local wastewater treatment plant (WWTP). MLVSS and OUR were measured in accordance with Standard Methods (APHA.%) for another 3 h. whereby the MBR was integrated with the RO process with a concentrate recycle stream. Samples taken from IMP for analyses include the wastewater. while another concentrate stream of the same flow rate was wasted through a bleed line. MBR effluent. TOC tests (TOC Analyzer. TDS levels (TDS Meter. 2000). ML supernatant. RO concentrate and RO permeate. As the RO element can only achieve a limited permeate recovery ratio of 10–15%.%). A chemical solution of EDTA (0. Membrane fouling resulted in a higher driving pressure to maintain a constant permeate flux.%) were used for organic cleaning while a citric acid solution (2.0 wt. NH3-N. The wastewater characteristics are shown in Table 1. As indicated by the standard deviation (SD).03 wt. in the wastewater and MBR effluent were both measured using the automated phenate method.6 psi. with pH adjusted to 4. was used for colloidal and inorganic cleaning. Phase 2 represented the operation of the MBR alone at a SRT of 20 days for 37 days. which were relatively stable. ML. When a 20 –30% increase in the required driving pressure was observed. Hanna Instruments) were measured for the wastewater.%) for 3 h followed by oxalic acid solution (0. The fouling layer formed on the membrane surfaces was removed by washing with a sponge and tap water. Phase 3 represented a transition period of 46 days.

Cww the wastewater TOC concentration (g/L).81 6. the average MBR TOC mass removal rate obtained in Phase 4 was higher than that of Phase 2. Ceff the MBR effluent TOC concentration (g/L). Throughout both phases. M4 the MBR TOC mass removal rate during Phase 4 (g/d).90 1. Only experimental data collected after this time period were analyzed. and QR the RO concentrate recycle stream flow rate (L/d). ML and effluent characteristics during Phases 2 and 4 Parameters Phase 2 Mean value 6 SD Phase 4 MLSS. mg/L ML TDS.282 ^ 191 20.72 ^ 2.hr ML DOC.61 7. It is noted that the trend line associated with Phase 4 was consistently above that of Phase 2 over the entire range of wastewater concentrations tested.54 12.12 ^ 0.H. experimental results obtained during Phases 2 and 4 were analyzed and compared. Qeff the MBR effluent flow rate (L/d). Qww the wastewater influent flow rate (L/d). mg/L TDS. Similar observation could also be seen from Figure 2 where the profiles of TOC mass removal rates during Phases 2 and 4 were plotted over a range of wastewater TOC concentrations. Effect of concentrate recycling on MBR mass removal rate As shown in Table 2.25 5.48 ^ 2.48 ^ 2. ML and effluent characteristics obtained in Phases 2 and 4. This finding indicated that concentrate recycling resulted in a higher TOC mass Table 2 Comparison of MBR TOC mass removal rate.Table 1 Characteristics of mixed municipal and industrial wastewater Wastewater characteristics Parameters Mean value 6 Standard deviation TOC. Table 3 summarizes the mean values and SD of both the RO concentrate and RO permeate characteristics obtained in Phase 4.49 945 ^ 89 458 C. mg/L MBR TOC mass removal rate. g/L sOUR.45 30.09 .19 37.47 ^ 3. M 2 ¼ C ww £ Qww 2 Ceff £ Qeff M 4 ¼ C ww £ Qww þ C R £ QR 2 Ceff £ Qeff ð1Þ ð2Þ where M2 is the MBR TOC mass removal rate during Phase 2 (g/d). ppm 110.61 ^ 53. g/d 10. Lew et al.53 ^ 1. mg/L NH3-N. allowing the biomass to be acclimated to the conditions of concentrate recycling. given by Eqs. nitrification was complete and no NH3-N was detected in the MBR effluent.44 ^ 2. CR the TOC concentration (g/L) of the RO concentrate recycle stream.86 ^ 0.19 10.22 922 ^ 73 14.75 ^ 2. ppm MBR effluent TOC. Table 2 summarizes the mean values and SD of the MBR TOC mass removal rates. A time period of 2 SRT was given for the stabilization of the MBR during Phase 4. (1) and (2).00 ^ 1.20 ^ 0.42 ^ 6.20 ^ 5. The performance of the MBR during Phases 2 and 4 was assessed and compared based on TOC mass removal rate. Results and discussion To investigate the effects of concentrate recycling on MBR performance.97 29. g/L MLVSS. mgO2/gVSS.92 8.68 6.

650 ^ 488 0. Lew et al. removal rate which in turn suggested that in addition to the residual readily degradable organic compounds. For both phases.53 3. the average MLSS and MLVSS concentrations were higher in Phase 4 than in Phase 2. a fraction of the slow.H. That is. These findings also suggested that the higher TOC mass removal rate was likely attributed to biodegradation. which shows the MLVSS concentrations over a range of wastewater TOC concentrations observed in Phases 2 and 4.811 ^ 0. Figure 2 Comparison of MBR TOC mass removal rate during Phases 2 and 4 at different wastewater TOC concentrations 459 .43 ^ 11. The increase in biomass concentration with substrate concentration indicated that a higher substrate concentration could support a higher level of growth which in turn suggested that there was insignificant inhibitory effect associated with concentrate recycling. The above claim can further be supported by the results presented in Table 2 whereby it could be seen that concentrate recycling did not result in any significant changes to the ML dissolved organic carbon (DOC) concentration.477 140 ^ 35 C. mg/L TDS.and-hard-to-degrade organic compounds present in the recycle stream could be biodegraded in the MBR. It should be highlighted that the trend line of Phase 4 was consistently above that of Phase 2.Table 3 RO concentrate and permeate characteristics during Phase 4 Parameters RO concentrate Mean value 6 SD RO permeate TOC. The higher ML DOC SD was attributed to the highly variable wastewater strength experienced in Phase 4. a higher biomass concentration was attainable due to the uptake and assimilation of additional substrates available in the concentrate recycle stream. ppm 56. There was also an observed increase in ML TDS concentration. the trend lines obtained indicated a corresponding increase in MLVSS concentration with the wastewater TOC concentration. Effect of concentrate recycling on MBR biomass concentration As shown in Table 2. These observations could be better illustrated in Figure 3. This finding could be attributed to the higher growth rate associated with Phase 4 that in turn facilitated a higher mass removal rate during phase 4. although it did not reach an inhibitory level. The higher SD could be attributed to the highly variable wastewater strength experienced during Phase 4. This phenomenon could be attributed to the high TDS concentration present in the recycle stream (Table 3).

four biodegradability batch tests were conducted. as compared with Batch test D. The type of substrate and source of biomass used for each batch test are summarized in Table 4. Batch test D.and hard-to-biodegrade in nature. Figure 4(b) compares the experimental results obtained from Batch tests A and B. ML from the MBR and WWTP were centrifuged and the resulting supernatant was discarded. Figure 3 Comparison of MLVSS concentrations during Phases 2 and 4 at different wastewater TOC concentrations Biodegradation batch tests To further validate the observation that a fraction of the slow. Autoclaving of biomass for batch test B was carried out at 121 8C for 20 mins. which used wastewater as the substrate. Batch test A. The DO level in the flasks was found to be above 4. After the addition of biomass to their respective substrates in conical flasks.5 g TOC/g VSS. This finding would suggest that bulk of the wastewater could be readily biodegraded.0 mg/L. As shown in Figure 4(a).460 C. Lew et al. the flasks were placed on a shaker operated at an rpm of 250. The four batch tests were operated at F/M ratios of around 0. followed by a more gradual decrease. The biomass was then washed twice by resuspension with phosphate buffer solution.45 mm filter papers.day. The filtrates were then measured for residual DOC. The much slower rate of residual DOC decrease observed in Batch test A. Samples were taken intermittently from the four batch tests by withdrawing 10 mL of ML from each flask before passing them through 0. showed a rapid decrease in DOC during the first hour. The aim of this comparison was to investigate the roles of biomass adsorption and biodegradation. B. It is noted from Figure 4(b) that Batch test B had a smaller decrease in DOC compared with Table 4 Substrate type and biomass source for Batch tests A. This preparation procedure allowed compounds adsorbed onto the biomass to be removed. which used RO concentrate as the substrate.and hard-to-degrade organic compounds present in the concentrate recycle stream could be degraded by an acclimated biomass. any decrease in residual DOC would be attributed to bioadsorption of concentrated constituents. In contrast. indicated that the bulk of the constituents in the RO concentrate were slow.H. C and D Batch test A B C D Substrate type Biomass source RO concentrate MBR RO concentrate MBR (autoclaved) RO concentrate WWTP Wastewater MBR . showed only a relatively small decrease in DOC. As the biomass used in Batch test B was washed and autoclaved. Figure 4 compares the variations of residual DOC with time for the four batch tests. Residual DOC of each batch test was monitored during a 5 h time period.

which used non-acclimated biomass. Effect of concentrate recycling on microbial viability and activity Assessment of microbial viability and activity was carried out based on sOUR measurements. C and D that attained by Batch test A. and that biomass adsorption was the main mechanism responsible for the decrease in DOC. 461 . B. the reduction in DOC associated with Batch test B was mainly attributed to biomass adsorption. did not show any observable biodegradation. It is noted from Figures 4(b) and 4(c) that the profile of residual DOC associated with Batch test C was similar to that of Batch test B. Figure 4(c) compares the experimental results obtained from Batch tests A and C. This finding suggested that there was minimal or no observable biodegradation occurring in Batch test C. This finding suggested that Phase 4 experienced a suppression of respiratory activities over the same range of F/M ratios compared with Phase 2. biodegradation only occurred in Batch test A where the biomass had been previously exposed and acclimated to conditions of concentrate recycling. In contrast. It is also noted that the trend line associated with Phase 4 was below that of Phase 2. Lew et al. This phenomenon could be attributed to the consequence of concentrate recycling. The “food” in all F/M ratios for Phase 4 was calculated based on the weighted concentration of the wastewater and the concentrate recycle stream. They accommodated the increase in F/M ratio via a corresponding increase in sOUR (during phase 4). The higher SD again could be explained by the highly variable wastewater strength experienced in Phase 4. SMP and wastewater inherent refractory compounds recycled back to the MBR had an inhibitory effect on the microorganisms. Although live biomass was used for both tests.C. the mean sOUR value obtained from Phase 4 was slightly less than that of Phase 2. which is crucial to the success of the novel IMP.and hard-to-degrade RO concentrate constituents. This finding indicated the importance of biomass acclimation to achieve biodegradation of slow. this inhibition was not severe and the microorganisms remained viable. This finding suggested that the microorganisms could accommodate the increase in substrate loading and the increase in loading led to a corresponding increase in oxygen uptake. It is also noted from Figure 5 that sOUR increased with F/M ratio. Batch test C.H. As shown in Table 2. However. This finding suggested that the reduction in DOC observed in Batch test A was attributed to both biomass adsorption and biodegradation. Figure 4 Comparisons of the variation of residual DOC with time for Batch tests A.

462 C.03 g TOC/g VSS. Lew et al. the effluent quality associated with Phase 4 was not significantly different from that obtained from Phase 2 whereby no concentrate recycling was implemented. For example. Figure 5 Comparison of sOUR during Phases 2 and 4 at different F/M ratios Effect of concentrate recycling on MBR effluent quality As shown in Table 2.H. as well as an increase in the concentration of the recycle stream. The deterioration of the effluent quality was more significant when F/M ratio was increased. with an F/M below 0. This observation can be better illustrated in Figure 6.day. However. the average MBR effluent TOC concentration associated with Phase 4 was higher than that of Phase 2. it should be pointed out that the increase in F/M ratio during Phase 4 was attributed to both an increase in the wastewater concentration. this drawback could be overcome by operating the MBR at a lower F/M ratio. It is noted from this figure that the MBR effluent TOC associated with Phase 2 deteriorated slightly as F/M ratio increased. which shows the relationship between effluent TOC concentrations and F/M ratios for Phases 2 and 4. This finding reflected the robustness of the MBR in terms of its ability to produce effluent of consistent quality even with varying wastewater strength. Although operating the MBR with a concentrate recycle stream resulted in an overall worsening of the effluent quality. However. such a trend was not observed when recycling of a concentrate stream was carried out. Figure 6 Comparisons of MBR effluent TOC trend during Phases 2 and 4 at different F/M ratio .

U. H. Water Research. J. Pound. CR the RO concentrate TOC concentration (g/L). and Kang. and David. Witzig. 463 .S. On the whole. A review of soluble microbial products (SMP) in wastewater treatment systems. Conclusions The novel IMP with concentrate recycling could deliver good performance in terms of overall TOC mass removal efficiency. Immersed membrane activated sludge for the reuse Co of municipal wastewater. Washington DC. the novel IMP had been demonstrated to achieve good overall TOC mass removal efficiency and was able to produce water of good quality for reuse purposes... and Stephenson.. References APHA (2000). G.. Liu.-S. (1999). Huang. 189 –196. H. and Arakaki.-T. Buisson. (1997). (2002). 601 – 610. Standard Methods for the Examination of Water and Wastewater. Duncan. Elsevier. K. Qperm the RO permeate flow rate (L/d).Performance of the novel IMP The performance of the novel IMP was assessed based on the overall TOC mass removal efficiency given by Eq. W. resulting in a slight suppression of respiratory activities. Yamamoto. (2003). C. C. The mean value and SD of MIMP were found to be 88. 49. where MIMP is the overall IMP TOC mass removal efficiency (%). Biotechnology and Bioengineering. K. (2000). M IMP ¼ C ww £ Qww 2 Cperm £ Qperm 2 CR £ QB £ 100% Cww £ Qww ð3Þ C. Performance of a Rosenberger. (2001). R. the recycled concentrate constituents had an inhibitory effect on the microorganisms. S. Behaviour of soluble microbial products in a membrane bioreactor. Kru bioreactor with submerged membranes for aerobic treatment of municipal wastewater.day could yield an effluent quality comparable to that achievable without implementing concentrate recycling. 401 –406. and Qian.. U. ¨ ger.80%. Amsterdam. Process Biochemistry.B. X. R. and Cww and Qww as previously defined. APHA/AWWA/WEF..94 ^ 3. 37.H. Cperm the RO permeate TOC concentration (g/L). However. Szewzyk. In: Advances in Water and Wastewater Treatment Technology. 33(14). ˆ te ´ .and hard-to-degrade organic constituents present in the recycle stream could be degraded by an acclimated biomass operating at a SRT of 20 days. Brindle. Characteristics and fates of soluble microbial products in ceramic membrane bioreactor at various sludge retention times. Thus.. 36. Desalination.03 g TOC/g VSS. USA. Water Research. Nonetheless. pp 229 – 237. Experimental results suggested that operating the MBR (in the novel IMP) at a F/M ratio below 0. P. S. 113. the inhibition was not severe and the microorganisms remained viable and responded to the increase in F/M ratio by a higher specific oxygen uptake rate. Water Research. The availability of additional substrates in the concentrate recycle stream could support a higher biomass growth that led to a higher biomass concentration. T. (3). QB the RO concentrate bleed rate (L/d). Membrane bioreactor: an advanced wastewater treatment/reclamation technology and its function in excess-sludge minimization. it has been demonstrated that the novel IMP could achieve good TOC mass removal efficiency and it is able to produce water of good quality for reuse purposes. The RO permeate quality is given in Table 3. 3063 –3082. 121 – 127. M. Shin. A portion of the slow. 413 – 420. (1996). Lew et al. The application of membrane biological reactors for the treatment of wastewater. and Kraume. Y. Manz. 36.