FeS自养反硝化与厌氧氨氧化的耦合脱氮机制
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摘要
微生物的功能多样性对元素价态的转换存在协同作用是自然界关键的生态调节策略,充分利用这种策略,实现不同微生物的功能组合,可以发展废水处理新工艺.本文以静态批次实验的含氮污染物作为研究对象,把Fe S投加量、NO_3~--N/NO_2~--N比值、厌氧氨氧化(ANAMMOX,AN)和自养反硝化(AD)生物量之比作为反应控制条件,讨论了AN与AD之间代谢产物互补的合作机制,提出了(AN+AD)_(TN→0)脱氮工艺的概念.研究发现过量的Fe S投加在保证AD过程的彻底性之外,并不显著影响AN菌的代谢活性;提高NO_2~--N在电子受体中的比例,会使微生物复合群落处于代谢底物竞争关系之中,对TN的去除产生负面影响; AN生物量的增加加深了复合群落的合作程度,当初始NH_4~+-N与NO_3~--N的化学计量比小于0. 85时,可以实现TN浓度趋零.结果表明,通过认识微生物之间的交互作用,寻求复杂微生物群落功能的规划或调控,可以设计出更加合理的废水处理工艺,达到低物耗投入条件下目标污染物的高效去除.
Synergy among members of complex microbial communities in the transformation of elements is a key ecological regulation strategy in nature. Making full use of this phenomenon and achieving functional combinations of different microorganisms may have a significant effect on developing new wastewater treatment processes. In this study,nitrogen-containing pollutants were applied in a static batch experiment. The dosage of Fe S,the ratio of NO_3~--N/NO_2~--N,and the ratio of ANAMMOX( AN) to autotrophic denitrification( AD) biomass were the controlled reaction conditions. The cooperation mechanism resulting from the metabolic complementation of AN and AD is discussed,and the concept of a( AN + AD)_(TN→0) nitrogen removal process is proposed. This study showed that the excessive dosage of Fe S could ensure the more thorough reaction of AD without significantly affecting the metabolic activity of AN bacteria. A complex microbial community was involved in the competition for metabolic substrates when the proportion of NO_2~--N in the electron acceptor was increased,resulting in a negative impact on the removal of TN. The increase of AN biomass contributed to the strengthening of the cooperation between AN and AD. When the stoichiometric ratio of NH_4~+-N to NO_3~--N was less than 0. 85,TN could be completely removed. The results showed that a more effective wastewater treatment process may be established by understanding the interactions between microorganisms,and by manipulating or regulating complex microbial communities. This could achieve the efficient removal of pollutants under low material consumption conditions.
Synergy among members of complex microbial communities in the transformation of elements is a key ecological regulation strategy in nature. Making full use of this phenomenon and achieving functional combinations of different microorganisms may have a significant effect on developing new wastewater treatment processes. In this study,nitrogen-containing pollutants were applied in a static batch experiment. The dosage of Fe S,the ratio of NO_3~--N/NO_2~--N,and the ratio of ANAMMOX( AN) to autotrophic denitrification( AD) biomass were the controlled reaction conditions. The cooperation mechanism resulting from the metabolic complementation of AN and AD is discussed,and the concept of a( AN + AD)_(TN→0) nitrogen removal process is proposed. This study showed that the excessive dosage of Fe S could ensure the more thorough reaction of AD without significantly affecting the metabolic activity of AN bacteria. A complex microbial community was involved in the competition for metabolic substrates when the proportion of NO_2~--N in the electron acceptor was increased,resulting in a negative impact on the removal of TN. The increase of AN biomass contributed to the strengthening of the cooperation between AN and AD. When the stoichiometric ratio of NH_4~+-N to NO_3~--N was less than 0. 85,TN could be completely removed. The results showed that a more effective wastewater treatment process may be established by understanding the interactions between microorganisms,and by manipulating or regulating complex microbial communities. This could achieve the efficient removal of pollutants under low material consumption conditions.
引文
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[10]Li X J,Sun S,Badgley B D,et al.Nitrogen removal by granular nitritation-anammox in an upflow membrane-aerated biofilm reactor[J].Water Research,2016,94:23-31.
[11]Ali M,Okabe S.Anammox-based technologies for nitrogen removal:advances in process start-up and remaining issues[J].Chemosphere,2015,141:144-153.
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[13]Li W,Li H,Liu Y D,et al.Salinity-aided selection of progressive onset denitrifiers as a means of providing nitrite for anammox[J].Environmental Science&Technology,2018,52(18):10665-10672.
[14]Wu L,Li Z,Zhao C,et al.A novel partial-denitrification strategy for post-anammox to effectively remove nitrogen from landfill leachate[J].Science of the Total Environment,2018,633:745-751.
[15]安芳娇,黄剑明,黄利,等.基质比对厌氧氨氧化耦合反硝化脱氮除碳的影响[J].环境科学,2018,39(11):5058-5064.An F J,Huang J M,Huang L et al.Effect of substrate ratio on removal of nitrogen and carbon using anaerobic ammonium oxidation and denitrification[J].Environmental Science,2018,39(11):5058-5064.
[16]Qin Y J,Cao Y,Ren J Y,et al.Effect of glucose on nitrogen removal and microbial community in anammox-denitrification system[J].Bioresource Technology,2017,244:33-39.
[17]Karanasios K A,Vasiliadou I A,Tekerlekopoulou A G,et al.Effect of C/N ratio and support material on heterotrophic denitrification of potable water in bio-filters using sugar as carbon source[J].International Biodeterioration&Biodegradation,2016,111:62-73.
[18]周健,黄勇,刘忻,等.硫自养反硝化耦合厌氧氨氧化脱氮条件控制研究[J].环境科学,2016,37(3):1061-1069.Zhou J,Huang Y,Liu X,et al.Element sulfur autotrophic denitrification combined anaerobic ammonia oxidation[J].Environmental Science,2016,37(3):1061-1069.
[19]Li X,Yuan Y,Huang Y,et al.Simultaneous removal of ammonia and nitrate by coupled S0-driven autotrophic denitrification and Anammox process in fluorine-containing semiconductor wastewater[J].Science of the Total Environment,2019,661:235-242.
[20]Zhu T T,Cheng H Y,Yang L H,et al.Coupled sulfur and iron(II)carbonate-driven autotrophic denitrification for significantly enhanced nitrate removal[J].Environmental Science&Technology,2019,53(3):1545-1554.
[21]Qian J,Zhang M K,Pei X J,et al.A novel integrated thiosulfate-driven denitritation(TDD)and anaerobic ammonia oxidation(anammox)process for biological nitrogen removal[J].Biochemical Engineering Journal,2018,139:68-73.
[22]Jin R C,Yang G F,Zhang Q Q,et al.The effect of sulfide inhibition on the ANAMMOX process[J].Water Research,2013,47(3):1459-1469.
[23]Gong Y Y,Tang J C,Zhao D Y.Application of iron sulfide particles for groundwater and soil remediation:a review[J].Water Research,2016,89:309-320.
[24]Wei Y Y,Dai J,Mackey H R,et al.The feasibility study of autotrophic denitrification with iron sludge produced for sulfide control[J].Water Research,2017,122:226-233.
[25]Lu H,Huang H Q,Yang W M,et al.Elucidating the stimulatory and inhibitory effects of dissolved sulfide on sulfuroxidizing bacteria(SOB)driven autotrophic denitrification[J].Water Research,2018,133:165-172.
[26]付炳炳,潘建新,马景德,等.采用含硫铁化学污泥作为反硝化电子供体进行焦化废水中总氮深度去除[J].环境科学,2018,39(7):3262-3270.Fu B B,Pan J X,Ma J D,et al.Evaluation of advanced nitrogen removal from coking wastewater using sulfide ironcontaining sludge as a denitrification electron donor[J].Environmental Science,2018,39(7):3262-3270.
[27]Pan J X,Ma J D,Wu H Z,et al.Application of metabolic division of labor in simultaneous removal of nitrogen and thiocyanate from wastewater[J].Water Research,2019,150:216-224.
[28]Van De Graaf A A,De Bruijn P,Robertson L A,et al.Autotrophic growth of anaerobic ammonium-oxidizing microorganisms in a fluidized bed reactor[J].Microbiology,1996,142(8):2187-2196.
[29]Gallegos T J,Hyun S P,Hayes K F.Spectroscopic investigation of the uptake of arsenite from solution by synthetic mackinawite[J].Environmental Science&Technology,2007,41(22):7781-7786.
[30]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.
[31]Lackner S,Terada A,Smets B F.Heterotrophic activity compromises autotrophic nitrogen removal in membrane-aerated biofilms:Results of a modeling study[J].Water Research,2008,42(4-5):1102-1112.
[32]Sun X B,Du L F,Hou Y Q,et al.Endogenous influences on anammox and sulfocompound-oxidizing autotrophic denitrification coupling system(A/SAD)and dynamic operating strategy[J].Bioresource Technology,2018,264:253-260.
[33]Shi Y,Hu S H,Lou J Q,et al.Nitrogen removal from wastewater by coupling anammox and methane-dependent denitrification in a membrane biofilm reactor[J].Environmental Science&Technology,2013,47(20):11577-11583.
[34]Strous M,Kuenen J G,Jetten M S M.Key physiology of anaerobic ammonium oxidation[J].Applied and Environmental Microbiology,1999,65(7):3248-3250.
[2]González-Martínez A,Calderón K,González-López J.New concepts of microbial treatment processes for the nitrogen removal:effect of protein and amino acids degradation[J].Amino Acids,2016,48(5):1123-1130.
[3]国家统计局,环境保护部.中国环境统计年鉴[M].北京:中国统计出版社,2016.
[4]Hooper A B,Vannelli T,Bergmann D J,et al.Enzymology of the oxidation of ammonia to nitrite by bacteria[J].Antonie Van Leeuwenhoek,1997,71(1-2):59-67.
[5]Arp D J,Sayavedra-Soto L A,Hommes N G.Molecular biology and biochemistry of ammonia oxidation by Nitrosomonas europaea[J].Archives of Microbiology,2002,178(4):250-255.
[6]Van Der Heijden R T J M,Heijnen J J,Hellinga C,et al.Linear constraint relations in biochemical reaction systems:I.Classification of the calculability and the balanceability of conversion rates[J].Biotechnology and Bioengineering,1994,43(1):3-10.
[7]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].Applied Microbiology and Biotechnology,1998,50(5):589-596.
[8]Ding S Z,Bao P,Wang B,et al.Long-term stable simultaneous partial nitrification,anammox and denitrification(SNAD)process treating real domestic sewage using suspended activated sludge[J].Chemical Engineering Journal,2018,339:180-188.
[9]Ma Y,Peng Y Z,Wang S Y,et al.Achieving nitrogen removal via nitrite in a pilot-scale continuous pre-denitrification plant[J].Water Research,2009,43(3):563-572.
[10]Li X J,Sun S,Badgley B D,et al.Nitrogen removal by granular nitritation-anammox in an upflow membrane-aerated biofilm reactor[J].Water Research,2016,94:23-31.
[11]Ali M,Okabe S.Anammox-based technologies for nitrogen removal:advances in process start-up and remaining issues[J].Chemosphere,2015,141:144-153.
[12]Du R,Cao S B,Li B K,et al.Performance and microbial community analysis of a novel DEAMOX based on partialdenitrification and anammox treating ammonia and nitrate wastewaters[J].Water Research,2017,108:46-56.
[13]Li W,Li H,Liu Y D,et al.Salinity-aided selection of progressive onset denitrifiers as a means of providing nitrite for anammox[J].Environmental Science&Technology,2018,52(18):10665-10672.
[14]Wu L,Li Z,Zhao C,et al.A novel partial-denitrification strategy for post-anammox to effectively remove nitrogen from landfill leachate[J].Science of the Total Environment,2018,633:745-751.
[15]安芳娇,黄剑明,黄利,等.基质比对厌氧氨氧化耦合反硝化脱氮除碳的影响[J].环境科学,2018,39(11):5058-5064.An F J,Huang J M,Huang L et al.Effect of substrate ratio on removal of nitrogen and carbon using anaerobic ammonium oxidation and denitrification[J].Environmental Science,2018,39(11):5058-5064.
[16]Qin Y J,Cao Y,Ren J Y,et al.Effect of glucose on nitrogen removal and microbial community in anammox-denitrification system[J].Bioresource Technology,2017,244:33-39.
[17]Karanasios K A,Vasiliadou I A,Tekerlekopoulou A G,et al.Effect of C/N ratio and support material on heterotrophic denitrification of potable water in bio-filters using sugar as carbon source[J].International Biodeterioration&Biodegradation,2016,111:62-73.
[18]周健,黄勇,刘忻,等.硫自养反硝化耦合厌氧氨氧化脱氮条件控制研究[J].环境科学,2016,37(3):1061-1069.Zhou J,Huang Y,Liu X,et al.Element sulfur autotrophic denitrification combined anaerobic ammonia oxidation[J].Environmental Science,2016,37(3):1061-1069.
[19]Li X,Yuan Y,Huang Y,et al.Simultaneous removal of ammonia and nitrate by coupled S0-driven autotrophic denitrification and Anammox process in fluorine-containing semiconductor wastewater[J].Science of the Total Environment,2019,661:235-242.
[20]Zhu T T,Cheng H Y,Yang L H,et al.Coupled sulfur and iron(II)carbonate-driven autotrophic denitrification for significantly enhanced nitrate removal[J].Environmental Science&Technology,2019,53(3):1545-1554.
[21]Qian J,Zhang M K,Pei X J,et al.A novel integrated thiosulfate-driven denitritation(TDD)and anaerobic ammonia oxidation(anammox)process for biological nitrogen removal[J].Biochemical Engineering Journal,2018,139:68-73.
[22]Jin R C,Yang G F,Zhang Q Q,et al.The effect of sulfide inhibition on the ANAMMOX process[J].Water Research,2013,47(3):1459-1469.
[23]Gong Y Y,Tang J C,Zhao D Y.Application of iron sulfide particles for groundwater and soil remediation:a review[J].Water Research,2016,89:309-320.
[24]Wei Y Y,Dai J,Mackey H R,et al.The feasibility study of autotrophic denitrification with iron sludge produced for sulfide control[J].Water Research,2017,122:226-233.
[25]Lu H,Huang H Q,Yang W M,et al.Elucidating the stimulatory and inhibitory effects of dissolved sulfide on sulfuroxidizing bacteria(SOB)driven autotrophic denitrification[J].Water Research,2018,133:165-172.
[26]付炳炳,潘建新,马景德,等.采用含硫铁化学污泥作为反硝化电子供体进行焦化废水中总氮深度去除[J].环境科学,2018,39(7):3262-3270.Fu B B,Pan J X,Ma J D,et al.Evaluation of advanced nitrogen removal from coking wastewater using sulfide ironcontaining sludge as a denitrification electron donor[J].Environmental Science,2018,39(7):3262-3270.
[27]Pan J X,Ma J D,Wu H Z,et al.Application of metabolic division of labor in simultaneous removal of nitrogen and thiocyanate from wastewater[J].Water Research,2019,150:216-224.
[28]Van De Graaf A A,De Bruijn P,Robertson L A,et al.Autotrophic growth of anaerobic ammonium-oxidizing microorganisms in a fluidized bed reactor[J].Microbiology,1996,142(8):2187-2196.
[29]Gallegos T J,Hyun S P,Hayes K F.Spectroscopic investigation of the uptake of arsenite from solution by synthetic mackinawite[J].Environmental Science&Technology,2007,41(22):7781-7786.
[30]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.
[31]Lackner S,Terada A,Smets B F.Heterotrophic activity compromises autotrophic nitrogen removal in membrane-aerated biofilms:Results of a modeling study[J].Water Research,2008,42(4-5):1102-1112.
[32]Sun X B,Du L F,Hou Y Q,et al.Endogenous influences on anammox and sulfocompound-oxidizing autotrophic denitrification coupling system(A/SAD)and dynamic operating strategy[J].Bioresource Technology,2018,264:253-260.
[33]Shi Y,Hu S H,Lou J Q,et al.Nitrogen removal from wastewater by coupling anammox and methane-dependent denitrification in a membrane biofilm reactor[J].Environmental Science&Technology,2013,47(20):11577-11583.
[34]Strous M,Kuenen J G,Jetten M S M.Key physiology of anaerobic ammonium oxidation[J].Applied and Environmental Microbiology,1999,65(7):3248-3250.