ANAMMOX体系中氨与硫酸盐的同步转化条件
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摘要
在CFSTR(continuous flow stirred tank reactor)反应器中接种混合污泥(ANAMMOX污泥与污水厂浓缩污泥按1∶1混合)研究NH_4~+与SO_4~(2-)的同步转化,通过不断投加污泥令体系内ORP值稳定在(-200±50) mV,同步转化现象持续42 d,NH_4~+平均转化14. 81 mg·L~(-1),SO_4~(2-)平均转化8. 77 mg·L~(-1).在批试实验中通过溶液是否充满玻璃瓶来控制体系内厌氧条件,不充满组NH_4~+与SO_4~(2-)均降低,但两者的转化不同步;在完全充满组中NH_4~+不转化,SO_4~(2-)浓度下降明显,实验后期检测到S~(2-).分析认为同步转化现象产生的一般条件为NH_4~+和SO_4~(2-)基质充足,接种浓度适量的混合污泥,体系漏氧且ORP检测值在-150～-300 mV范围内.同时认为本文及相关研究中所使用的实验条件均不能证明NH_4~+与SO24-的同步转化是两者相互转化的结果,相反实验条件更利于NH4+与SO24-各自独立转化.
A continuous flow stirred tank reactor( CFSTR) was used to inoculate mixed sludge( with an ANAMMOX sludge to sewage concentrate sludge ratio of 1: 1) to study the simultaneous conversion of NH_4~+and SO_4~(2-). The ORP value in the system was stabilized at(-200 ± 50) m V by continuously adding sludge. The simultaneous conversion lasted for 42 days. The average conversion of NH_4~+-N was 14. 81 mg·L~(-1) while that of sulfate-sulfur was 8. 77 mg·L~(-1). In the batch experiment,the anaerobic conditions were influenced by whether the solution was filled with glass bottles. Both NH_4~+and SO_4~(2-) in the non-filled group were reduced,but their transformation was not simultaneous. In the fully filled group,NH_4~+was not transformed,the concentration of SO_4~(2-) decreased significantly,and S~(2-)was detected in the later stages of the experiment. It is indicated that the general conditions for the phenomenon of simultaneous conversion are: ①sufficient NH_4~+and SO_4~(2-),② inoculating mixed sludge with appropriate concentration,③ leaking oxygen,④ the detection value of ORP within the range of-150 to-300 mV. At the same time,the experimental conditions used in this paper and in other related literature cannot prove that the simultaneous conversion of NH_4~+and SO_4~(2-)is the result of mutual transformation; on the contrary,observations are more conducive to the independent transformation of NH_4~+and SO_4~(2-).
A continuous flow stirred tank reactor( CFSTR) was used to inoculate mixed sludge( with an ANAMMOX sludge to sewage concentrate sludge ratio of 1: 1) to study the simultaneous conversion of NH_4~+and SO_4~(2-). The ORP value in the system was stabilized at(-200 ± 50) m V by continuously adding sludge. The simultaneous conversion lasted for 42 days. The average conversion of NH_4~+-N was 14. 81 mg·L~(-1) while that of sulfate-sulfur was 8. 77 mg·L~(-1). In the batch experiment,the anaerobic conditions were influenced by whether the solution was filled with glass bottles. Both NH_4~+and SO_4~(2-) in the non-filled group were reduced,but their transformation was not simultaneous. In the fully filled group,NH_4~+was not transformed,the concentration of SO_4~(2-) decreased significantly,and S~(2-)was detected in the later stages of the experiment. It is indicated that the general conditions for the phenomenon of simultaneous conversion are: ①sufficient NH_4~+and SO_4~(2-),② inoculating mixed sludge with appropriate concentration,③ leaking oxygen,④ the detection value of ORP within the range of-150 to-300 mV. At the same time,the experimental conditions used in this paper and in other related literature cannot prove that the simultaneous conversion of NH_4~+and SO_4~(2-)is the result of mutual transformation; on the contrary,observations are more conducive to the independent transformation of NH_4~+and SO_4~(2-).
引文
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[10]Liu S T,Yang F L,Gong Z,et al.Application of anaerobic ammonium-oxidizing consortium to achieve completely autotrophic ammonium and sulfate removal[J].Bioresource Technology,2008,99(15):6817-6825.
[11]Yang Z Q,Zhou S Q,Sun Y B.Start-up of simultaneous removal of ammonium and sulfate from an anaerobic ammonium oxidation(anammox)process in an anaerobic up-flow bioreactor[J].Journal of Hazardous Materials,2009,169(1-3):113-118.
[12]秦永丽,蒋永荣,刘成良,等.硫酸盐型厌氧氨氧化反应器的启动特性[J].环境工程学报,2015,9(12):5849-5854.Qin Y L,Jiang Y R,Liu C L,et al.Starting characteristics of sulfate-dependent anaerobic ammonium oxidation reactor[J].Chinese Journal of Environmental Engineering,2015,9(12):5849-5854.
[13]马文娟,赵东风,刘春爽,等.pH值促进硫酸盐型厌氧氨氧化的快速启动[J].化学与生物工程,2015,32(10):17-20.Ma W J,Zhao D F,Liu C S,et al.Fast start-up of sulfate ANAMMOX promoted by p H value[J].Chemistry&Bioengineering,2015,32(10):17-20.
[14]赖杨岚,周少奇.硫酸盐型厌氧氨氧化反应器的启动特征分析[J].中国给水排水,2010,26(15):41-44.Lai Y L,Zhou S Q.Start-up characteristics of sulfate-dependent anaerobic ammonium oxidation reactor[J].China Water&Wastewater,2010,26(15):41-44.
[15]刘正川,袁林江,周国标,等.从亚硝酸还原厌氧氨氧化转变为硫酸盐型厌氧氨氧化[J].环境科学,2015,36(9):3345-3351.Liu Z C,Yuan L J,Zhou G B,et al.Achievement of sulfatereducing anaerobic ammonium oxidation reactor started with nitrate-reducting anaerobic ammonium oxidation[J].Environmental Science,2015,36(9):3345-3351.
[16]Prachakittikul P,Wantawin C,Noophan P,et al.ANAMMOX-like performances for nitrogen removal from ammonium-sulfaterich wastewater in an anaerobic sequencing batch reactor[J].Journal of Environmental Science and Health,Part A:Toxic/Hazardous Substances and Environmental Engineering,2016,51(3):220-228.
[17]张蕾,郑平,何玉辉,等.硫酸盐型厌氧氨氧化性能的研究[J].中国科学B辑:化学,2008,38(12):1113-1119.Zhang L,Zheng P,He Y H,et al.Performance of sulfatedependent anaerobic ammonium oxidation[J].Science in China Series B:Chemistry,2009,52(1):86-92.
[18]蒋永荣,秦永丽,刘可慧.粉煤灰对硫酸盐型厌氧氨氧化驯化过程的影响[J].生态环境学报,2016,25(8):1387-1394.Jiang Y R,Qin Y L,Liu K H.The effect of fly ash on domestication of sulfate-dependent anaerobic ammonium oxidation[J].Ecology and Environmental Sciences,2016,25(8):1387-1394.
[19]李祥,黄勇,袁怡,等.自养厌氧硫酸盐还原/氨氧化反应器启动特性[J].化工学报,2012,63(8):2606-2611.Li X,Huang Y,Yuan Y,et al.Starting characteristics of a reactor for simultaneous reduction of sulfate and oxidation of ammonium[J].CIESC Journal,2012,63(8):2606-2611.
[20]袁怡,黄勇,李祥,等.硫酸盐还原-氨氧化反应的特性研究[J].环境科学,2013,34(11):4362-4369.Yuan Y,Huang Y,Li X,et al.Characteristics of sulfate reduction-ammonia oxidation reaction[J].Environmental Science,2013,34(11):4362-4369.
[21]Yuan Y,Huang Y,Li X,et al.Characteristics of sulfate reduction-ammonia oxidation under anaerobic conditions[J].Journal of Residuals Science&Technology,2015,12:115-121.
[22]张丽,黄勇,袁怡,等.硫酸盐/氨的厌氧生物转化试验研究[J].环境科学,2013,34(11):4356-4361.Zhang L,Huang Y,Yuan Y,et al.Study on the biotransformation of sulfate and ammonia in anaerobic conditions[J].Environmental Science,2013,34(11):4356-4361.
[23]刘福鑫,黄勇,袁怡,等.厌氧硫酸盐还原-氨氧化的研究[J].环境工程学报,2015,9(2):699-704.Liu F X,Huang Y,Yuan Y,et al.Study of anaerobic sulfatereducing ammonium oxidation reaction[J].Chinese Journal of Environmental Engineering,2015,9(2):699-704.
[24]王慧.硫酸盐型厌氧氨氧化同步脱氮除硫实验研究[D].沈阳:沈阳工业大学,2017.Wang H.Study on sulfate-reducing ANAMMOX reaction for synchronizing ammonia and sulfate removal[D].Shenyang:Shenyang University of Technology,2017.
[25]完颜德卿,黄勇,毕贞,等.硫酸盐还原氨氧化体系中基质转化途径[J].环境科学,2017,38(8):3406-3414.Wanyan D Q,Huang Y,Bi Z,et al.Conversion pathways of substrates in sulfate-reducing ammonia oxidation system[J].Environmental Science,2017,38(8):3406-3414.
[26]国家环境保护总局.水和废水监测分析方法[M].(第四版).北京:中国环境科学出版社,2002.
[27]闵航,陈美慈,赵宇华,等.厌氧微生物学[M].杭州:浙江大学出版社,1993.164-166.
[28]蒋永荣,秦永丽,刘可慧.粉煤灰对硫酸盐型厌氧氨氧化驯化过程的影响[J].生态环境学报,2016,25(8):1387-1394.Jiang Y R,Qin Y L,Liu K H.The effect of fly ash on domestication of sulfate-dependent anaerobic ammonium oxidation[J].Ecology and Environmental Sciences,2016,25(8):1387-1394.
[29]Zhang Z,Liu S.Insight into the overconsumption of ammonium by ANAMMOX consortia under anaerobic conditions[J].Journal of Applied Microbiology,2014,117(6):1830-1838.
[30]国际水协(IWA)良好建模实践工作组(GMP).活性污泥模型应用指南[M].施汉昌,胡志荣,杨殿海,等译.北京:中国建筑工业出版社,2015.201-202.
[31]孙培德,宋英琦,王如意.活性污泥动力学模型及数值模拟导论[M].北京:化学工业出版社,2010.44-45.
[32]高廷耀,顾国维,周琪.水污染控制工程-下册[M].(第三版).北京:高等教育出版社,2007.124-173.
[33]刘建丽,赵吉,武琳慧.乌梁素海湖滨湿地硫酸盐还原菌群落多样性及系统发育分析[J].安全与环境学报,2016,16(3):343-348.Liu J L,Zhao J,Wu L H.Analysis for the sulfate-reducing bacteria in the littoral wetland around the beach area of Wuliangsuhai Lake[J].Journal of Safety and Environment,2016,16(3):343-348.
[2]van de Graaf A A,Mulder A,de Bruijn P,et al.Anaerobic oxidation of ammonium is a biologically mediated process[J].Applied and Environmental Microbiology,1995,61(4):1246-1251.
[3]van der Star W R L,Abma W R,Blommers D,et al.Startup of reactors for anoxic ammonium oxidation:experiences from the first full-scale anammox reactor in Rotterdam[J].Water Research,2007,41(18):4149-4163.
[4]Tang C J,Zheng P,Wang C H,et al.Performance of highloaded ANAMMOX UASB reactors containing granular sludge[J].Water Research,2011,45(1):135-144.
[5]Yang W H,Weber K A,Silver W L.Nitrogen loss from soil through anaerobic ammonium oxidation coupled to iron reduction[J].Nature Geoscience,2012,5(8):538-541.
[6]Javanaud C,Michotey V,Guasco S,et al.Anaerobic ammonium oxidation mediated by Mn-oxides:from sediment to strain level[J].Research in Microbiology,2011,162(9):848-857.
[7]Sumino T,Isaka K,Ikuta H,et al.Nitrogen removal from wastewater using simultaneous nitrate reduction and anaerobic ammonium oxidation in single reactor[J].Journal of Bioscience and Bioengineering,2006,102(4):346-351.
[8]Strous M,Kuenen J G,Fuerst J A,et al.The anammox case-a new experimental manifesto for microbiological eco-physiology[J].Antonie van Leeuwenhoek,2002,81(1-4):693-702.
[9]Fdz-Polanco F,Fdz-Polanco M,Fernandez N,et al.New process for simultaneous removal of nitrogen and sulphur under anaerobic conditions[J].Water Research,2001,35(4):1111-1114.
[10]Liu S T,Yang F L,Gong Z,et al.Application of anaerobic ammonium-oxidizing consortium to achieve completely autotrophic ammonium and sulfate removal[J].Bioresource Technology,2008,99(15):6817-6825.
[11]Yang Z Q,Zhou S Q,Sun Y B.Start-up of simultaneous removal of ammonium and sulfate from an anaerobic ammonium oxidation(anammox)process in an anaerobic up-flow bioreactor[J].Journal of Hazardous Materials,2009,169(1-3):113-118.
[12]秦永丽,蒋永荣,刘成良,等.硫酸盐型厌氧氨氧化反应器的启动特性[J].环境工程学报,2015,9(12):5849-5854.Qin Y L,Jiang Y R,Liu C L,et al.Starting characteristics of sulfate-dependent anaerobic ammonium oxidation reactor[J].Chinese Journal of Environmental Engineering,2015,9(12):5849-5854.
[13]马文娟,赵东风,刘春爽,等.pH值促进硫酸盐型厌氧氨氧化的快速启动[J].化学与生物工程,2015,32(10):17-20.Ma W J,Zhao D F,Liu C S,et al.Fast start-up of sulfate ANAMMOX promoted by p H value[J].Chemistry&Bioengineering,2015,32(10):17-20.
[14]赖杨岚,周少奇.硫酸盐型厌氧氨氧化反应器的启动特征分析[J].中国给水排水,2010,26(15):41-44.Lai Y L,Zhou S Q.Start-up characteristics of sulfate-dependent anaerobic ammonium oxidation reactor[J].China Water&Wastewater,2010,26(15):41-44.
[15]刘正川,袁林江,周国标,等.从亚硝酸还原厌氧氨氧化转变为硫酸盐型厌氧氨氧化[J].环境科学,2015,36(9):3345-3351.Liu Z C,Yuan L J,Zhou G B,et al.Achievement of sulfatereducing anaerobic ammonium oxidation reactor started with nitrate-reducting anaerobic ammonium oxidation[J].Environmental Science,2015,36(9):3345-3351.
[16]Prachakittikul P,Wantawin C,Noophan P,et al.ANAMMOX-like performances for nitrogen removal from ammonium-sulfaterich wastewater in an anaerobic sequencing batch reactor[J].Journal of Environmental Science and Health,Part A:Toxic/Hazardous Substances and Environmental Engineering,2016,51(3):220-228.
[17]张蕾,郑平,何玉辉,等.硫酸盐型厌氧氨氧化性能的研究[J].中国科学B辑:化学,2008,38(12):1113-1119.Zhang L,Zheng P,He Y H,et al.Performance of sulfatedependent anaerobic ammonium oxidation[J].Science in China Series B:Chemistry,2009,52(1):86-92.
[18]蒋永荣,秦永丽,刘可慧.粉煤灰对硫酸盐型厌氧氨氧化驯化过程的影响[J].生态环境学报,2016,25(8):1387-1394.Jiang Y R,Qin Y L,Liu K H.The effect of fly ash on domestication of sulfate-dependent anaerobic ammonium oxidation[J].Ecology and Environmental Sciences,2016,25(8):1387-1394.
[19]李祥,黄勇,袁怡,等.自养厌氧硫酸盐还原/氨氧化反应器启动特性[J].化工学报,2012,63(8):2606-2611.Li X,Huang Y,Yuan Y,et al.Starting characteristics of a reactor for simultaneous reduction of sulfate and oxidation of ammonium[J].CIESC Journal,2012,63(8):2606-2611.
[20]袁怡,黄勇,李祥,等.硫酸盐还原-氨氧化反应的特性研究[J].环境科学,2013,34(11):4362-4369.Yuan Y,Huang Y,Li X,et al.Characteristics of sulfate reduction-ammonia oxidation reaction[J].Environmental Science,2013,34(11):4362-4369.
[21]Yuan Y,Huang Y,Li X,et al.Characteristics of sulfate reduction-ammonia oxidation under anaerobic conditions[J].Journal of Residuals Science&Technology,2015,12:115-121.
[22]张丽,黄勇,袁怡,等.硫酸盐/氨的厌氧生物转化试验研究[J].环境科学,2013,34(11):4356-4361.Zhang L,Huang Y,Yuan Y,et al.Study on the biotransformation of sulfate and ammonia in anaerobic conditions[J].Environmental Science,2013,34(11):4356-4361.
[23]刘福鑫,黄勇,袁怡,等.厌氧硫酸盐还原-氨氧化的研究[J].环境工程学报,2015,9(2):699-704.Liu F X,Huang Y,Yuan Y,et al.Study of anaerobic sulfatereducing ammonium oxidation reaction[J].Chinese Journal of Environmental Engineering,2015,9(2):699-704.
[24]王慧.硫酸盐型厌氧氨氧化同步脱氮除硫实验研究[D].沈阳:沈阳工业大学,2017.Wang H.Study on sulfate-reducing ANAMMOX reaction for synchronizing ammonia and sulfate removal[D].Shenyang:Shenyang University of Technology,2017.
[25]完颜德卿,黄勇,毕贞,等.硫酸盐还原氨氧化体系中基质转化途径[J].环境科学,2017,38(8):3406-3414.Wanyan D Q,Huang Y,Bi Z,et al.Conversion pathways of substrates in sulfate-reducing ammonia oxidation system[J].Environmental Science,2017,38(8):3406-3414.
[26]国家环境保护总局.水和废水监测分析方法[M].(第四版).北京:中国环境科学出版社,2002.
[27]闵航,陈美慈,赵宇华,等.厌氧微生物学[M].杭州:浙江大学出版社,1993.164-166.
[28]蒋永荣,秦永丽,刘可慧.粉煤灰对硫酸盐型厌氧氨氧化驯化过程的影响[J].生态环境学报,2016,25(8):1387-1394.Jiang Y R,Qin Y L,Liu K H.The effect of fly ash on domestication of sulfate-dependent anaerobic ammonium oxidation[J].Ecology and Environmental Sciences,2016,25(8):1387-1394.
[29]Zhang Z,Liu S.Insight into the overconsumption of ammonium by ANAMMOX consortia under anaerobic conditions[J].Journal of Applied Microbiology,2014,117(6):1830-1838.
[30]国际水协(IWA)良好建模实践工作组(GMP).活性污泥模型应用指南[M].施汉昌,胡志荣,杨殿海,等译.北京:中国建筑工业出版社,2015.201-202.
[31]孙培德,宋英琦,王如意.活性污泥动力学模型及数值模拟导论[M].北京:化学工业出版社,2010.44-45.
[32]高廷耀,顾国维,周琪.水污染控制工程-下册[M].(第三版).北京:高等教育出版社,2007.124-173.
[33]刘建丽,赵吉,武琳慧.乌梁素海湖滨湿地硫酸盐还原菌群落多样性及系统发育分析[J].安全与环境学报,2016,16(3):343-348.Liu J L,Zhao J,Wu L H.Analysis for the sulfate-reducing bacteria in the littoral wetland around the beach area of Wuliangsuhai Lake[J].Journal of Safety and Environment,2016,16(3):343-348.