Two-Stage Anaerobic Fluidized-Bed Membrane Bioreactor Treatment of Settled Domestic Wastewater J. Bae*, R. Yoo*, E. Lee* and P. L. McCarty*, ** * Department of Environmental Engineering, Inha University, Namgu, Yonghyun dong 253, Incheon, Republic of Korea (E-mail: [email protected]; [email protected]; [email protected]) ** Department of Civil and Environmental Engineering, Stanford University, Stanford, CA 94305, USA (E-mail: [email protected]) Abstract A two-stage anaerobic fluidized-bed membrane bioreactor (SAF-MBR) system was applied for the treatment of primary-settled domestic wastewater that was further pre-treated by either 10 µm filtration or 1 mm screening. While the different pre-treatment options resulted in different influent qualities, the effluent qualities were quite similar. In both cases at a total hydraulic retention time (HRT) of 2.3 hr and 25oC, COD and BOD5 removals were 84%-91% and 92%-94%, with effluent concentrations lower than 25 and 7 mg/L, respectively. With a membrane flux of 6-12 L/m2/h, trans-membrane pressure (TMP) remained below 0.2 bar during 310 days of continuous operation without need for membrane chemical cleaning or backwashing. Biosolids production was estimated to be 0.028-0.049 g VSS/g BOD5, which is far less than that with comparable aerobic processes. Electrical energy production from combined heat and power utilization of the total methane produced (gaseous and dissolved) was estimated to be more than sufficient for total system operation. Keywords: anaerobic fluidized bed bioreactor; membrane; sewage treatment INTRODUCTION Anaerobic treatment of sewage would be a good alternative to aerobic processes with the advantages of energy recovery and low sludge production. Although poor effluent quality has often been found to be a problem with anaerobic treatment of domestic wastewater (Gomec, 2010; Seghezzo et al., 2007), this can be overcome using a membrane bioreactor, which can capture effluent suspended solids and maintain a long solids retention time (SRT). However, membrane fouling has been a major barrier to its application with high operating and energy costs (Smith et. al., 2012). Many attempts have been made to reduce membrane fouling (Alan et al., 2010; Huang et al., 2011; Martinez-Sosa et al., 2011). Kim et al. (2011) recently proposed a novel staged fluidized bed membrane bioreactor (SAF-MBR) system consisting of an anaerobic fluidized bed reactor (AFBR) and an anaerobic fluidized membrane bioreactor (AFMBR) in series. When continuously fed 500 mg/L COD synthetic wastewater at 35oC with a total hydraulic retention time (HRT) of 5.0 hr, overall COD removal was 99%, with permeate COD of 7±4 mg/L. The clogging of the membrane was successfully controlled by the scouring effect of granular activated carbon (GAC) in the AFMBR, with less energy consumption compared to a submerged membrane bioreactor using gas sparging for fouling control. In a subsequent study, Yoo et al. (2012) evaluated this system at 25oC using primary settled domestic wastewater that was subsequently screened with a 10 µm filter, and found similar treatment results. The objective of this study was to further evaluate the performance of the SAF-MBR system for treatment of domestic wastewater at ambient temperature. The study by Yoo et al. (2012) using 10 µm filtered settled domestic wastewater was extended for an additional 100 days using a more practical settled domestic wastewater that was screened with a 1 mm screen, yielding a total study time for the SAF-MBR of 310 days with the same membranes. Concern has been expressed over the impact of GAC fluidization on membrane integrity (Smith et al., 2012), and so evaluation of long-term membrane operation is of importance. In this study, organic removal efficiency, biosolids production, and energy balance were evaluated while operating the SAF-MBR system without the use of membrane chemical cleaning or backwashing. MATERIALS AND METHODS Reactor operation The lab-scale SAF-MBR system illustrated in Figure 1 has been described in detail by Yoo et al. (2012). The 0.245 L AFBR contained 30 g of 10 x 30 mesh fresh GAC as support medium for bacterial growth. The AFMBR was the same size, but contained 54 g of fresh GAC and a submerged membrane module consisting of eight 0.45 m long, polyvinylidenefluoride (PVDF) hollow fiber membranes, with surface area of 0.0215 m2. Fluidization of GAC was maintained with a magnetic pump to maintain the desired recirculation flow rate (Table 1). Gas bag Gas bag Overflow line Peristaltic pump Sludge wasting line 100 % expension Peristaltic pump 40 % expension Pressure gauge Peristaltic pump Permeate Flow meter Flow meter Recirculation pump - AFBR - Influent Recirculation pump - AFMBR - Figure 1. Schematic diagram of the SAF-MBR system (after Yoo et al., 2012) The SAF-MBR system was operated at 25oC under two different Modes based on the pre-treatment of feed wastewater as summarized in Table 1. Details of operation under Mode I was reported previously (Yoo et al., 2012). A summary of that data is also presented here in order to compare with the new results presented here on Mode II operation. The feed to the treatment system was primary effluent from a sewage treatment plant in Bucheon, Korea, which was taken once a week and stored under 4oC refrigeration. Just prior to use, the wastewater was filtered through either a 10 m cartridge filter (Mode I) or a 1 mm screen (Mode II). With 10 m filtration about 60% of the primary effluent total suspended solids (TSS) were removed. However, with 1 mm screening, TSS rejection was negligible, and thus the feed wastewater was close in composition to the primary effluent. The SAF-MBR system was operated at a set-point permeate flux of 6 to 9 LMH for 98 days before Mode I, which lasted for 61 days. Between Modes I and II, the SAF-MBR was operated for 51 days to determine the sustainable flux that could be maintained without producing significant membrane fouling, which was 11 LMH (Yoo et al., 2012). Then Mode II operation was begun and lasted for 100 days. For both Modes I and II the HRT of the AFBR and the AFMBR were 1.0 and 1.3 hr, respectively. The corresponding membrane flux of the AFMBR for these two Modes was maintained at 9 L/m2/h (LMH). About 280 ml of recycle fluid was withdrawn each week to remove excess suspended biosolids production for disposal. The organic loading rate (OLR) of the AFBR increased from 3.7 kg COD/m3-d (Mode I) to 5.6 kg COD/m3-d (Mode II), an increase caused by the higher feed VSS during Mode II. Table 1. Operating conditions for Modes I and II for the SAF-MBR system Mode I Mode II AFBR Operating period (days) Influent pre-treatment AFBR AFMBR 61 100 10 ㎛ filtration 1 mm screen 25 25 Temperature (oC) HRT (h) AFMBR 1.0 1.3 1.0 1.3 - 9 - 9 OLR (kg COD/m3-d) 3.7 1.3 5.6 1.2 Recirculation flow rate (L/d) 446 1008 504 1080 Membrane flux (LMH) Analytical procedures COD, BOD5, total and volatile suspend solids (TSS, VSS), pH and alkalinity were determined according to procedures in Standard Methods (APHA, 1998). Sulfate was analyzed with an ionchromatograph (DX 500, Dionex, Sunnyvale, CA, USA) and volatile fatty acids (VFA) were analyzed with a HP 6890 series gas chromatograph with flame ionization detector (FID). Biogas production was measured using a gas bag (TDC, Japan) for collection. Gas composition was determined using a GC with thermal conductivity detector (HP6890 series Gas Chromatograph, Hewlett–Packard, USA). Dissolved methane was also measured with a method described in more detail elsewhere (Shin et al., 2011). RESULTS AND DISCUSSION Organic removal and effluent quality Table 2 contains a summary of the performance of the AFBR, the AFMBR, and the overall SAFMBR system. In Mode I, the AFBR achieved a COD removal of 56%, while the AFMBR reduced its influent COD by an additional 63%, providing an overall COD removal for the two-stage system of 84%. Although influent COD in Mode II was higher than that in Mode I, effluent COD slightly decreased from 25 mg/L (Mode I) to 22 mg/L (Mode II). As a result, COD removal in the AFBR increased to 72%, resulting in the overall COD removal of 91%. The average effluent BOD5 values were below 7 mg/L in both Modes, and corresponding BOD5 removal efficiencies were equal to or higher than 92%. Effluent volatile fatty acids were 3 mg COD/L or less, indicating almost complete degradation. Table 2. Performance of SAF-MBR system COD VSS VFA 154±34 88±23 40±7 37±7 - Eff. (mg/L) 68±18 25±9 21±7 18±4 4±4 AFMBR Eff. (mg/L) 25±10 7±2 2±1 2±1 3±3 Overall Rem. (%) 84 92 94 95 - Inf. (mg/L) 235±44 105±28 93±27 78±23 - Eff. (mg/L) 66±12 30±10 21±7 19±7 1±1 AFMBR Eff. (mg/L) 22±8 6±2 1±0 1±0 1±1 Overall Rem. (%) 91 94 99 99 - AFBR Mode II TSS Inf. (mg/L) AFBR Mode I BOD5 Some organics were removed by sulphate reduction. Influent sulphate concentration was relatively constant throughout the study with an average value of 64 mg/L, complete removal of which is equivalent to the removal of 42.5 mg COD/L. Thus, sulphate reduction not only reduces methane production potential but also causes a need for sulphide control in both the liquid and gas phases. The relatively higher COD removal in Mode II than Mode I was associated both with the increase in influent volatile suspended solids (VSS) and its subsequent greater removal in the AFBR from 51% (Mode I) to 76% (Mode II). Reasons for the higher removal during AFBR treatment during Mode II are not clear. Perhaps this resulted from better attachment of VSS on the AFBR GAC biofilm during Mode II and build-up or subsequent degradation there, the development of organisms with better VSS degradation capabilities, or because the larger VSS present were themselves more readily biodegradable. Effluent VSS concentrations in both Modes were near zero through membrane filtration. The pH and alkalinity varied over the range of 6.75-7.30 and 225-275 mg/L as CaCO3, respectively. The above results indicate that the SAF-MBR system can produce effluent quality meeting some of the stricter organic discharge requirements. VSS reduction and biosolids production In order to quantify VSS reduction and biosolids production, changes in total biomass accumulation within the reactors, including the attached biomass on GAC particles need to be considered. However, measurement of biomass accumulation on the GAC particles is not easy to perform without upsetting reactor operation. It was measured once for both reactors, 260 and 239 days after the start-up of the AFBR and the AFMBR, respectively, time periods ranging between the Mode I and II periods of operation (Yoo et al., 2012). Estimated total biomass at these later dates on the GAC particles was 1.11 g VSS in the AFBR and 0.58 g in the AFMBR, corresponding respectively to accumulations of 0.71 and 0.50 mg VSS/L as listed in Table 3. VSS destruction summarized in Table 3 indicates that the AFBR provided an increased VSS destruction capacity with high influent VSS, 19 mg VSS/L in Mode I, to 59 mg VSS/L in Mode II. On the other hand, VSS destruction in the AFMBR remained constant at 13-15 mg VSS/L. The removal of excess VSS from the SAF-MBR system was accomplished by weekly removal of the recycle fluid from the AFMBR (280 mL/week) and by a period removal that occurred during pump and recycle line cleaning. Based on the measured concentration of VSS in the wasting stream, wasting from the AFMBR was estimated to be 1.11 mg VSS/L, while that with pump and recycle line cleaning was 1.64 mg/L. The resulting net total biosolids production estimate including both biomass accumulation on GAC and VSS wasting was 0.049 g VSS/g BOD5 removed or 0.031 g VSS/g COD removed (Yoo et al, 2012). However, the biofilm growth could be ruled out from this calculation as most growth on the GAC probably occurred early during reactor start-up and not during Mode I. With this assumption, net total biosolids production estimate (Table 3) was 0.034 g VSS/g BOD5 removed or 0.021 g VSS/g COD removed in Mode I. The true biosoilds production would lie between the two values. In Mode II, the respective values decreased to 0.028 g VSS/g BOD5 removed and 0.013 g VSS/g COD removed. Table 3. Removal, wasting, and destruction of VSS during Modes I and II of operation Mode I Mode II Units : mg/L (unless otherwise specified) AFBR AFMBR Total AFBR AFMBR Total Removal 19 16 35 Bulk solution 1.11 Recirculation line & pump Totals 59 18 77 1.11 0.84 0.84 1.64 1.64 1.91 1.91 2.75 2.75 2.75 2.75 Wasting Destruction 19 13 32 59 15 74 % of reactor influent 49 72 84 76 79 95 The above biosolids production is far less than the typical value for aerobic secondary sewage treatment of 0.42 g VSS/g BOD5 (Rittman and McCarty, 2001), or for an aerobic fluidized bed reactor of 0.12-0.135 g VSS /g COD (Patel, et al., 2006). For an anaerobic fluidized bed reactor, Borja et al, (2000) reported a biomass yield of 0.075 g VSS/g COD, while Jovanovic et al. (1986) indicated a net VSS yield of 0.03 g VSS/g COD with an operating OLR of 20 kg COD/m3-d. The biosolids production in the SAF-MBR system was slightly lower than these reported anaerobic values, perhaps because the AFMBR was aided by its provision of a longer SRT. Membrane fouling control by GAC fluidization The AFMBR was operated continuously for 310 days without the need for cleaning procedures such as backwashing or chemical washing, and with low trans-membrane pressure (TMP) as illustrated in Figure 2. This long-term fouling free operation resulted from the scouring effect of the fluidized GAC (Kim et al., 2011). Before Mode I, the AFMBR was operated for 98 days at a flux of 6 LMH, and the TMP remained below 0.1 bar. During Mode I, TMP was maintained in the narrow range of 0.042 and 0.057 bar for 61 days. After Mode I operation, the maximum sustainable flux of the AFMBR was tested over a 51 day period. This was found to be about 11 LMH using a variety of on and off procedures. The flux of 9 LMH used throughout Mode I was then selected as the best for longer-term operation and the Mode II evaluation. With this flux during Mode II an average TMP of 0.116±0.015 bar was obtained. Mode I Mode II 0.4 TMP (bar) 0.3 0.2 0.1 0.0 0 50 100 150 200 250 300 Time (d) Figure 2. TMP variations for the AFMBR during 310 days of operation. Energy consideration Table 4 contains an electrical energy balance for the system, calculated as described by Yoo et al. (2012). This considers all energy transfer efficiencies between pumps, motors, and generators. The energy requirement was similar for both Modes. Electrical energy requirement for the pump for fluidization of GAC was the major energy requirement, and was 0.011 and 0.036 kWh/m3 for the AFBR and AFMBR, respectively. The three times greater energy requirement for the AFMBR than for the AFBR was due to the need for full fluidization of GAC to cover the membranes in the AFMBR. Also, a small additional electrical energy requirement of 0.001 kWh/m3 was needed for the AFMBR permeate pump. The total estimated electrical energy requirement for system operation during Modes I and II was 0.048 and 0.053 kWh/m3, respectively. During Mode II, the estimated electrical energy that could be obtained from gaseous and dissolved methane was 0.034 and 0.064 kWh/m3, respectively, or somewhat higher than during Mode I. Therefore in Mode II, with gaseous methane only, about 64% of the energy requirement could be satisfied. With the recovery of dissolved methane, the SAF-MBR system may become an energy self-sufficient process. Even if not used as an energy source, it is important that dissolved methane be captured or otherwise destroyed in some manner as it is a strong greenhouse gas. Commercial systems such as gas stripping or gas-permeable membrane processes are available and can be used Table 4. Estimated energy balance for the SAF-MBR system Units : kWh/m3 (unless otherwise indicated) Mode I Mode II AFBR AFMBR Total AFBR AFMBR Total 0.011 0.036 0.047 0.012 0.037 0.051 0.001 0.001 0.003 0.002 0.037 0.048 0.012 0.040 0.053 0.009 0.030 0.023 0.011 0.034 0.052 0.052 0.064 0.064 0.061 0.082 0.075 0.098 Electrical Energy required for GAC fluidization for permeate production Total 0.011 Energy production potential from Methane Gaseous 0.021 Dissolved Total 0.021 0.023 Energy produced/required With gaseous methane 63% 64% With total methane 174% 188% to recover the dissolved methane. The above analysis does not include the electrical energy potential of the methane produced form primary treatment, which if included should make the SAFMBR system a significant net producer of electrical energy. CONCLUSIONS The SAF-MBR system was applied for the treatment of a primary-settled domestic wastewater at 25oC and a total HRT of 2.3 h. The effluent quality was similar whether the settled wastewater was pre-treated using 10 m filtration or 1 mm screening, as the increased VSS concentration with screening was mostly removed in the first stage AFBR. Overall COD and BOD5 were 84%-91% and 92%-94% removed with permeate concentrations lower than 25 and 7 mg/L, respectively. For 310 days of operation, no membrane fouling control, such as chemical cleaning or backwashing, was needed other than that resulting from the souring effect of the fluidized GAC particles. Electrical energy that could result from combustion of the total methane produced (gaseous and dissolved) would be more than sufficient for total system operation. Biosolids production was estimated to be 0.028-0.049 g VSS/g BOD5, which is far less than that from comparable aerobic processes. The SAF-MBR system has good potential as a low-energy highefficiency cost-effective domestic wastewater treatment system. 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