部分亚硝化—厌氧氨氧化耦合工艺处理污泥脱水液的研究
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摘要
污泥脱水液属于低碱度、低C/N、高氨氮废水,采用传统的生物硝化/反硝化工艺已不能满足这类低C/N、高氨氮废水的处理要求。因此开发应用型高效、低耗的生物脱氮工艺显得尤为重要,亚硝化、厌氧氨氧化(ANAMMOX)、全程自养脱氮等新型生物脱氮技术的研究成为当前的研究热点。然而,目前的研究成果大多处于实验室配水研究阶段。
本试验以实际污泥脱水液为研究对象,采用缺氧滤床+好氧悬浮填料生物膜连续流工艺,在常温、高溶解氧条件下,于好氧反应器中实现和维持了脱水液部分亚硝化;同时采用先启动硝化生物膜再启动ANAMMOX应器的方法,成功启动了ANAMMOX反应器,然后将部分亚硝化反应器和ANAMMOX反应器耦合起来,进而实现全程自养生物脱氮,达到高效生物脱氮目的。此耦合工艺具有无需外加有机碳源、节省需氧量、降低能耗等优点。
本试验主要结果如下:
在高溶解氧(6～9mg/L)、常温(15～29℃)、长SRT条件下,利用特定抑制因子游离氨(FA)对亚硝酸盐氧化菌的抑制作用,从而使氨氧化菌在数量或活性上占优势,成功地在缺氧滤床+好氧悬浮填料生物膜连续流工艺中实现了部分亚硝化。在亚硝化反应器启动前130d过程中FA浓度在1.0～10.3mg/L,均在抑制亚硝酸盐氧化菌活性的阈值范围内。长期维持FA的选择性抑制作用,从而获得稳定的亚硝化,亚硝氮积累率可达80%左右,当进水氨氮有机负荷(ALR)为1.15 kg/(m3·d)时,亚硝氮积累率高达97.7%。通过综合调控进水ALR、进水碱度/氨氮和好氧段水力停留时间,可以调节出水NO2--N/NH4+-N的比率。当进水NH4+-N平均为315.8mg/L,平均进水ALR为0.43 kg/(m3·d),进水碱度/氨氮为5.25时,出水NO2--N/NH4+-N为1.25左右,从而为ANAMMOX工艺创造了进水条件,较好地实现了匹配ANAMMOX工艺的部分亚硝化。
采用先培养自养硝化生物膜,再启动ANAMMOX反应器的方法,可以在110d内快速启动厌氧氨氧化。第200d时反应器的NH4+-N和NO2--N去除容积负荷分别为0.526kg/(m3·d)和0.536kg/(m3·d)。在启动初期,由于好氧氨氧化占主导地位,出水pH值低于进水pH值。随着启动过程的推进,厌氧氨氧化逐渐占主导地位,出水pH值高于进水。第110～200d,氨氮去除量、NO2--N去除量、NO3--N生成量的比值平均为1:1.1:0.33。在ANAMMOX反应器的启动过程中,通过反应器内NH4+-N去除量、NO2--N去除量、NO3--N生成量及它们之间的比值、进出水pH值的变化作为指示参数,可以及时了解厌氧氨氧化的启动进程。生物膜启动厌氧氨氧化的反应器在提高ANAMMOX菌的固定化、减少菌种流失方面具有较大优势。
部分亚硝化反应器出水NO2--N/NH4+-N比率对提高该耦合工艺的脱氮效率至关重要,当进水NH4+-N为640mg/L,ALR为1.16kg/m3·d,进水碱度/氨氮为5.1时,进入ANAMMOX反应器的NO2--N/NH4+-N为1.2左右时,ANAMMOX反应器TN去除率可达83.8%。在不需外加有机碳源的条件下,处理高氨氮、碱度不足、低C/N实际污泥脱水液,实现了高效自养脱氮。本耦合工艺是适合污泥脱水液水质特点的新型生物脱氮技术。
Sludge liquor, which is characterized by high concentration of ammonium、low alkalinity and low C/N ratio. The conventional biological nitrification-denitrification cannot to achieve the processing request for this kind of waste water. Therefor it is important that researching and developing new nitrogen removal biotechnology. In resent years, the new biotechnologies such as ANAMMOX (Anaerobic Ammonium Oxidation), NITRITATION, CANON process have been the focus of research all around the world. Whereas the most new nitrogen removal processes have been limited in laboratory scale.
The sludge liquor was studied in this paper. The partial nitrification was achieved and and maintained stably in the aerobic carrier biofilm reactor under normal temperature and the high DO. At the same time, the ANAMMOX bioreactor can be started-up by cultivating autotrophic nitrifying biofilm first. The combine the nitritation reactor and the ANAMMOX reactor to achieve the completely autotrophic nitrogen removal over bitrite. The coupling process has advantages of no need of organic carbon addition, low oxygen consumption and energy consumption.
The main results were as follows:
The partial nitrification was achieved and maintained stably in the aerobic reactor under normal temperature(15～29℃)、the high DO(6～9mg/L) and long SRT, by the selective inhibition action of free ammonia to nitrite oxidation bacteria. The partial nitrification maintained stably in the aerobic reactor and nitration was about eighty percent when FA concentration was in the range of 1.0～10.3mg/L, in the 130 days prior to operation of the process. The nitration up to 97.7% when the influent ammonia loading rate(ALR) was 1.15 kg/m3·d. The effluent nitrite/ammonia ratio was about 1.25 when the average influent ammonia, influent ALR and influent ratio of alkalinity and ammonia were 315.80mg/L, 0.43 kg/m3·d and 5.25, respectively. So the effluent of partial nitrification process provided the influent substrate demand for the following ANAMMOX process.
The start-up of the ANAMMOX bioreactor by autotrophic nitrifying biofilm was studied. The ANAMMOX bioreactor can be initiated within 110 days when cultivating autotrophic nitrifying biofilm before the start-up of the bioreactor. At the 200th day, the volumetric loading rates of NH4+-N and NO2--N are 0.526 kg/m3·d and 0.536 kg/m3·d respectively. At the beginning of the start-up phase, the effluent pH value is lower than the influent pH value, but gradually, the effluent pH becomes higher than the influent pH value as the pH value of the liquid in the bioreactor is alkaline. Between the 110th and 200th day, the ratio of the NH4+-N removal, the NO2--N removal and the NO3--N production is 1:1.1:0.33. In the start-up course of ANAMMOX bioreactor, by the variation of the ratio of the NH4+-N removal and the NO2--N removal and the NO3--N production, the effluent and influent pH can demonstrate the start-up progression of the bioreactor. Besides, the ANAMMOX bioreactor has greater advantages at improving the immobilized of ANAMMOX bacteria and reducing the outflow of bacteria.
The effluent nitrite/ammonia ratio has a vital role to improve nitrogen removal efficiency of couping process. When influent ALR and alkalinity/ammonia ratio were respectively 1.16 kg/m3·d and 5.1, effluent ratioof nitrite to ammonia of the nitritation reactor was about 1.2 and total nitrogen removal efficiency of the ANAMMOX reactor was about 83.8%. The couping process achieved autotrophic nitrogen removal and without adding organic carbon source, so the noval adapt to water characteristics of digested sludge liquor.
本试验以实际污泥脱水液为研究对象,采用缺氧滤床+好氧悬浮填料生物膜连续流工艺,在常温、高溶解氧条件下,于好氧反应器中实现和维持了脱水液部分亚硝化;同时采用先启动硝化生物膜再启动ANAMMOX应器的方法,成功启动了ANAMMOX反应器,然后将部分亚硝化反应器和ANAMMOX反应器耦合起来,进而实现全程自养生物脱氮,达到高效生物脱氮目的。此耦合工艺具有无需外加有机碳源、节省需氧量、降低能耗等优点。
本试验主要结果如下:
在高溶解氧(6～9mg/L)、常温(15～29℃)、长SRT条件下,利用特定抑制因子游离氨(FA)对亚硝酸盐氧化菌的抑制作用,从而使氨氧化菌在数量或活性上占优势,成功地在缺氧滤床+好氧悬浮填料生物膜连续流工艺中实现了部分亚硝化。在亚硝化反应器启动前130d过程中FA浓度在1.0～10.3mg/L,均在抑制亚硝酸盐氧化菌活性的阈值范围内。长期维持FA的选择性抑制作用,从而获得稳定的亚硝化,亚硝氮积累率可达80%左右,当进水氨氮有机负荷(ALR)为1.15 kg/(m3·d)时,亚硝氮积累率高达97.7%。通过综合调控进水ALR、进水碱度/氨氮和好氧段水力停留时间,可以调节出水NO2--N/NH4+-N的比率。当进水NH4+-N平均为315.8mg/L,平均进水ALR为0.43 kg/(m3·d),进水碱度/氨氮为5.25时,出水NO2--N/NH4+-N为1.25左右,从而为ANAMMOX工艺创造了进水条件,较好地实现了匹配ANAMMOX工艺的部分亚硝化。
采用先培养自养硝化生物膜,再启动ANAMMOX反应器的方法,可以在110d内快速启动厌氧氨氧化。第200d时反应器的NH4+-N和NO2--N去除容积负荷分别为0.526kg/(m3·d)和0.536kg/(m3·d)。在启动初期,由于好氧氨氧化占主导地位,出水pH值低于进水pH值。随着启动过程的推进,厌氧氨氧化逐渐占主导地位,出水pH值高于进水。第110～200d,氨氮去除量、NO2--N去除量、NO3--N生成量的比值平均为1:1.1:0.33。在ANAMMOX反应器的启动过程中,通过反应器内NH4+-N去除量、NO2--N去除量、NO3--N生成量及它们之间的比值、进出水pH值的变化作为指示参数,可以及时了解厌氧氨氧化的启动进程。生物膜启动厌氧氨氧化的反应器在提高ANAMMOX菌的固定化、减少菌种流失方面具有较大优势。
部分亚硝化反应器出水NO2--N/NH4+-N比率对提高该耦合工艺的脱氮效率至关重要,当进水NH4+-N为640mg/L,ALR为1.16kg/m3·d,进水碱度/氨氮为5.1时,进入ANAMMOX反应器的NO2--N/NH4+-N为1.2左右时,ANAMMOX反应器TN去除率可达83.8%。在不需外加有机碳源的条件下,处理高氨氮、碱度不足、低C/N实际污泥脱水液,实现了高效自养脱氮。本耦合工艺是适合污泥脱水液水质特点的新型生物脱氮技术。
Sludge liquor, which is characterized by high concentration of ammonium、low alkalinity and low C/N ratio. The conventional biological nitrification-denitrification cannot to achieve the processing request for this kind of waste water. Therefor it is important that researching and developing new nitrogen removal biotechnology. In resent years, the new biotechnologies such as ANAMMOX (Anaerobic Ammonium Oxidation), NITRITATION, CANON process have been the focus of research all around the world. Whereas the most new nitrogen removal processes have been limited in laboratory scale.
The sludge liquor was studied in this paper. The partial nitrification was achieved and and maintained stably in the aerobic carrier biofilm reactor under normal temperature and the high DO. At the same time, the ANAMMOX bioreactor can be started-up by cultivating autotrophic nitrifying biofilm first. The combine the nitritation reactor and the ANAMMOX reactor to achieve the completely autotrophic nitrogen removal over bitrite. The coupling process has advantages of no need of organic carbon addition, low oxygen consumption and energy consumption.
The main results were as follows:
The partial nitrification was achieved and maintained stably in the aerobic reactor under normal temperature(15～29℃)、the high DO(6～9mg/L) and long SRT, by the selective inhibition action of free ammonia to nitrite oxidation bacteria. The partial nitrification maintained stably in the aerobic reactor and nitration was about eighty percent when FA concentration was in the range of 1.0～10.3mg/L, in the 130 days prior to operation of the process. The nitration up to 97.7% when the influent ammonia loading rate(ALR) was 1.15 kg/m3·d. The effluent nitrite/ammonia ratio was about 1.25 when the average influent ammonia, influent ALR and influent ratio of alkalinity and ammonia were 315.80mg/L, 0.43 kg/m3·d and 5.25, respectively. So the effluent of partial nitrification process provided the influent substrate demand for the following ANAMMOX process.
The start-up of the ANAMMOX bioreactor by autotrophic nitrifying biofilm was studied. The ANAMMOX bioreactor can be initiated within 110 days when cultivating autotrophic nitrifying biofilm before the start-up of the bioreactor. At the 200th day, the volumetric loading rates of NH4+-N and NO2--N are 0.526 kg/m3·d and 0.536 kg/m3·d respectively. At the beginning of the start-up phase, the effluent pH value is lower than the influent pH value, but gradually, the effluent pH becomes higher than the influent pH value as the pH value of the liquid in the bioreactor is alkaline. Between the 110th and 200th day, the ratio of the NH4+-N removal, the NO2--N removal and the NO3--N production is 1:1.1:0.33. In the start-up course of ANAMMOX bioreactor, by the variation of the ratio of the NH4+-N removal and the NO2--N removal and the NO3--N production, the effluent and influent pH can demonstrate the start-up progression of the bioreactor. Besides, the ANAMMOX bioreactor has greater advantages at improving the immobilized of ANAMMOX bacteria and reducing the outflow of bacteria.
The effluent nitrite/ammonia ratio has a vital role to improve nitrogen removal efficiency of couping process. When influent ALR and alkalinity/ammonia ratio were respectively 1.16 kg/m3·d and 5.1, effluent ratioof nitrite to ammonia of the nitritation reactor was about 1.2 and total nitrogen removal efficiency of the ANAMMOX reactor was about 83.8%. The couping process achieved autotrophic nitrogen removal and without adding organic carbon source, so the noval adapt to water characteristics of digested sludge liquor.
引文
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61 D. Zeqin, S. Tieheng. A Potential New Process for Improveing Nitrogen Removal in Constructed Wetlands-Promoting Coexistence of Partial-Nitrification and ANAMMOX[J]. Ecological Engineering, 2007, 31:69-78
62 L. Zhu, L. Junxin. Landfill Leachate Treatment with a Novel Process: Anaerobic Anammox Oxidation(Anammox) Combined with Soil Infiltration System[J]. Journal of Hazardous Materials, In Press, Corrected Proof, Available online 31 May 2007
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64 Van Dongen U, Jetten M S M, Van Loosdrecht M C M. The SHARON-Anammox Process for treatment of ammonium rich wastewater[J]. Wat Sci Tech,2001,44(1):153-160
65 Fux C, Boehler M, Huber P, Brunner I, Siegrist H. Biological treatment of ammonium-rich wastewater by partial nitrogen and subsequent anaerobic ammonium oxidation(anammox) in a pilot plant[J]. J Biotachnol,2002,99(3):295-306
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67 H. Siegrist. Nitrogen removal from digester supernatants-comparison of chemical and biological methods. Water Science Technology,1996,34(1～2):399-406
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66 P. Battistoni, P. Pavan, F. Cecchni., etc. Phosphorus removal in real anaerobic supernatants: modeling and performance of a fluidized bed reactor. Water Science Technology, 1998,38(1):275-283
67 H. Siegrist. Nitrogen removal from digester supernatants-comparison of chemical and biological methods. Water Science Technology,1996,34(1～2):399-406
68 Villaverde S, Garc a–Encina P A, Fdz–Polanco F. Influence of pH over nitrifying biofilm activity in sumerged biofilers [J]. Wat Res, 1997, 31(5): 1180-1186
69 Surmacz-Gorska J, Cichon A, Miksch K. Nitrogen removal from wastewater with high ammonia nitrogen concentration via shorter a nitrification and denitrification [J]. Wat Sci Tech,1997, 36(10): 73-78
70 Hellinga C, Schellen A A J C, Mulder J W, et al. The SHARON process: an innovative method for nitrogen removal from ammonia–rich waste water [J]. Wat Sci Tech, 1998, 37(9): 135-142
71 Munch E V, Lant P, Keller J. Simultaneous nitrification and denitrification in bench–scale sequencing batch reactors [J]. Wat Res, 1996, 30(2): 277-284
72 Balmelle B, Nguyen M, Capdeville B, et al. Study of factors controlling nitrite build-up in biological processes for water nitrification [J]. Wat Sci Tech, 1992, 26(5–6) :1017-1025
73 Mulder J. W., Rogier van Kempen. N-removal by SHARON. IAWQ Coference, 1997.30-31
74高景峰. SBR法去除有机物和脱氮除磷在线模糊控制的基础研究[D].哈尔滨:哈尔滨工业大学, 2001. 193-194
75 Hanaki K, Wantawin C, Ohgaki S. Nitrification at low levels of dissolved oxygen with and without organic loading in a suspended-growth reactor. Wat Res, 1990, 24(3): 297-302
76 Hagopian D S, Riley J G. A closer look at the bacteriology of nitrification [J]. Aquacultural Engineering, 1998, 18(4): 223-244
77 Anthonisen A C, Loehr R C, Prakasam T B S, et al. Inhibition of nitrification by ammonia and nitrous acid[J]. J. Water Pollut. Control Fed., 1976, 48(5): 835-852
78徐冬梅,聂梅生,金承基.亚硝酸型硝化的试验研究.给水排水, 1999, 25(7): 37-39
79陈际达,陈志胜,张光辉,等.含氮废水亚硝化型硝化的研究[J ] .重庆大学学报(自然科学版), 2000, 23(3): 74-76
80左剑恶,杨洋,蒙爱红.高氨氮浓度下的亚硝化过程及其影响因素研究.环境污染与防治, 2003, 25(6): 332-335
81魏琛,罗固源.游离氨对稳定生物亚硝化的影响分析.重庆环境科学, 2003, 25(12): 50-52
82 Wang Jianlong, Yang Ning. Partial nitrification under limited dissolved oxygen conditions[J]. Process Biochemistry, 2004, 39(10):1223-1229
83 Strous M, Heijnen J J, Kuenen J G, et al. The sequencing batch reactor as a powerful tool for the study of slowly growing anaerobic ammonium-oxidizing microorganisms[J]. Appl. Microbiol. Biotechnol., 1998, 50(5): 589-596
84 Schmid M, Twachtmann U, Klein M, et al. Molecular evidence for genus level diversity of bacteria capable of catalyzing anaerobic ammonium oxidation[J]. Sys. Appl. Microbiology., 2000, 23(1): 93-106
85 Van de Graaf A A, De Bruijn P, Robertson L A, et al. Autotrophic growth of anaerobic ammonium-oxidizing micro-organisms in a fluidized bed reactor[J]. Microbiology, 1996, 142(8): 2187-2196
86 Bock EI, Stueven R, Zart D. Nitrogen loss caused by denitrifying nitrosomonas cells using ammonium or hydrogen as electron donors and nitrite as electron acceptor. Arch Microbial, 1995, 163: 16-20
87张少辉,郑平,华玉妹.反硝化生物膜启动厌氧氨氧化反应器的研究[J].环境科学学报, 2004, 24(2): 220-224
88杜兵,司亚安,孙艳玲,等. ANAMMOX微生物高负荷培养方法研究[J].给水排水, 2004, 30(10): 35
89 Strous M, Kuenen J G, Jetten M S M. Key physiology of anaerobic ammonium oxidation[ J ]. Appl Environ. Microbiol, 1999, 65 (7) : 3248 - 3250
90 Jetten M S M, Strous M, van de Pas Schoonen K T, et al. The anaerobic oxidation of ammonium [ J ]. FEMS Microbiol Rev, 1999, 22 (5) : 421 - 437
91杜兵,司亚安,孙艳玲,等.推流固定化生物反应器培养ANAMMOX菌.中国给水排水, 2003, 19(7):62~65
92 Schmidt I, Sliekers O, Schmid M, et al. Aerobic and anaerobic ammonia oxidizing bacteria-competitors or natural partners[J]. FEMS Microbiology Ecology, 2002, 39(3): 175-181
93 Sliekers A O, Derwort N, Campos Gomez J L, et al. Completely autotrophic nitrogen removal over nitrite in one single reactor[J]. Water Research, 2002, 36(10): 2475-2482
94 Egli K, Fanger U, Alvarez P J J, et al. Enrichment and characterization of an anammox bacterium from a roating biological contactor treating ammonium-rich leachate[J]. Archives of Microbiology, 2001, 175(3): 198-207
95 Van de Graaf A A, De Bruijn P, Robertson L A, et al. Autotrophlic growth of anaerobic ammonium-oxidizing microorganisms in a fluidized bed reactor[J]. Microbiology,1996,142(8):2187-2196
96 Lindsay M R, Webb R I, Strous M, et al. Cell compartmentalization in planctomycetes: novel types of structural organization for the bacterial cell. Arch. Microbiol.,2001,175(6): 413-429
97郝晓地,仇付国, Van der Star W R L, Van Loosdrecht M C M.厌氧氨氧化技术工程化的全球现状及展望[J].中国给水排水, 2007, 23(18): 15-19
98 Van der Star W R L, Abma W R, Blommers D, et al. Start up of reactors for anoxic ammonium oxidation: experiences from the first full scale ANAMMOX reactor in Rotterdam [J]. Water Research,2007, 41(18):4149-4163
99郑平,徐向阳,胡宝兰.新型生物脱氮理论与技术[M].北京:科学出版社,2004: 155-165