微生物燃料电池降解焦化废水过程研究
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摘要
焦化废水生化处理流程复杂,污染物降解过程尚不明确,构建无膜空气阴极焦化废水微生物燃料电池,利用循环伏安法、红外分析、微生物群落结构等分析考察了焦化废水的降解过程中,各类有机物含量变化、官能团的变化、有机物异步降解次序及优势菌种的演替.焦化废水中含硫无机物被优先降解,酚类降解次之,含氮污染物历经好氧硝化与厌氧反硝化降解过程,但落后于前者;长链烷烃类降解缓慢;生物群落结构与底物中有机物种类密切相关,初期Desulfurella优先氧化含硫污染物、Flavobacterium降解酚类次之、Nitrospirae氧化降解NH_4~+-N较为缓慢,随时间延长Alcaligenes、Thiobacillus演变为优势菌落,实现了酚类的降解及NO_3~-的反硝化降解;电池输出电压为470.9mV,最高输出功率密度达12.5mW/cm2,COD、Tphenols、Tsurful、TN、NH_4~+-N的降解分别为85.8%、83.3%、87.5%、43.8%、89.9%.利用微生物燃料电池技术处理焦化废水,一步实现水质净化及能量回收,为废水生物处理控制提供理论和实践参考.
The current biological process for coking wastewater treatment requires the combination of several units with different methods.In addition,the mechanism of how the pollutants would be degraded along the whole plant is still not yet defined.All these consequently prevent targeted optimization to be conducted.To tackle these problems,a membrane-less air-cathode microbial fuel cell was constructed in this paper.Cyclic voltammetry and polarization were carried out to characterize the electrochemical performance of MFCs,while infrared spectroscopy,colorimetric methods and pyrosequencing were applied to trace the changes of chemicals and microbial communities in the reactor during the batch.The results revealed that sulfur-containing inorganic compounds in coking wastewater were degraded at the first,followed by the degradation of phenols.After that,nitrogen-containing pollutants were then removed through a combined pathway of aerobic nitrification and anaerobic denitrification.The degradation of long chain alkanes happened at the later phase of the batch.In addition,it was found that the microbial community structure was highly dependent on the available nutrients presented in the liquid phase.Desulfurella and Flavobacterium were dominant in the community in the early stage to perform aerobic decomposition of sulfurous and phenol pollutants,which would be latterly taken over by Nitrospitrae,Alcaligenes and Thiobacillus for nitrification and denitrification.The maximum power density of the MFC achieved was 12.5 mW/cm~2,of which the cell voltage was 470.9 mV.The total removal efficiencies of COD,TPhenols,Tsulfur,TN and NH_4~+-N were 85.8%,83.3%,87.5%,43.8% and 89.9%,respectively.All these data demonstrated the feasibility of a one-step process for coking wastewater treatment using microbial fuel cell.
The current biological process for coking wastewater treatment requires the combination of several units with different methods.In addition,the mechanism of how the pollutants would be degraded along the whole plant is still not yet defined.All these consequently prevent targeted optimization to be conducted.To tackle these problems,a membrane-less air-cathode microbial fuel cell was constructed in this paper.Cyclic voltammetry and polarization were carried out to characterize the electrochemical performance of MFCs,while infrared spectroscopy,colorimetric methods and pyrosequencing were applied to trace the changes of chemicals and microbial communities in the reactor during the batch.The results revealed that sulfur-containing inorganic compounds in coking wastewater were degraded at the first,followed by the degradation of phenols.After that,nitrogen-containing pollutants were then removed through a combined pathway of aerobic nitrification and anaerobic denitrification.The degradation of long chain alkanes happened at the later phase of the batch.In addition,it was found that the microbial community structure was highly dependent on the available nutrients presented in the liquid phase.Desulfurella and Flavobacterium were dominant in the community in the early stage to perform aerobic decomposition of sulfurous and phenol pollutants,which would be latterly taken over by Nitrospitrae,Alcaligenes and Thiobacillus for nitrification and denitrification.The maximum power density of the MFC achieved was 12.5 mW/cm~2,of which the cell voltage was 470.9 mV.The total removal efficiencies of COD,TPhenols,Tsulfur,TN and NH_4~+-N were 85.8%,83.3%,87.5%,43.8% and 89.9%,respectively.All these data demonstrated the feasibility of a one-step process for coking wastewater treatment using microbial fuel cell.
引文
[1]陈长松,李天增,张宝林,等.A/O工艺处理焦化废水的工程实践[J].环境科学与技术,2006,10(29):85-87.
[2]杨平,王彬,石炎福,等.生物流化床A-A-O工艺处理焦化废水中试研究[J].化工学报,2002,10(53):1085-1088.
[3]林琳,李玉平,曹宏斌,等.焦化废水厌氧氨氧化生物脱氮的研究[J].中国环境科学,2010,30(9):1201-1206.
[4]张伟,韦朝海,彭平安,等.A/O/O生物流化床处理焦化废水中酚类组成及降解特性分析[J].环境工程学报,2010,2(4):253-257.
[5]徐庆荣,包胜,蔡建安.厌氧/好氧/缺氧(A/O/A)工艺处理焦化废水的试验研究[J].净水技术,2011,30(1):39-41.
[6]Shi S,Qu Y,Ma Q,et al.Performance and microbial community dynamics in bioaugmented aerated filter reactor treating with coking wastewater[J].Bioresource Technology,2015,190:159-166.
[7]柏耀辉,孙庆华,赵翠,等.焦化废水处理系统中喹啉降解菌的种群特征[J].中国环境科学,2008,28(5):449-455.
[8]蒙小俊,李海波,盛宇星,等.焦化废水活性污泥PAH双加氧酶基因多样性分析[J].中国环境科学,2017,37(1):367-372.
[9]唐海,徐建平,安东,等.TiO2/ZSM-5m光催化耦合过硫酸盐降解焦化尾水的研究[J].中国环境科学,2015,35(11):3325-3332.
[10]Kent T D,S.C.Williams BSc MIChemE,Fitzpatrick C S B.Ammoniacal Nitrogen Removal in Biological Aerated Filters:The Effect of Media Size[J].Water&Environment Journal,2010,14(6):409-414.
[11]Qiu Y L,Hanada S,Ohashi A,et al.Syntrophorhabdus aromaticivorans gen.nov.sp.nov.the first cultured anaerobe capable of degrading phenol to acetate in obligate syntrophic associations with a hydrogenotrophic methanogen[J].Applied&Environmental Microbiology,2008,74(7):2051.
[12]郭楚玲,郑天凌.多环芳烃的微生物降解与生物修复[J].海洋环境科学,2000,19(3):24-29.
[13]吴黄英,周培疆,黄强盛.以木质纤维素生物质为降解底物的微生物燃料电池[J].武汉大学学报(理学版),2016,4(32):307-312.
[14]汪家权,夏雪兰,丁巍巍.微生物燃料电池处理苯酚废水运行条件研究[J].环境科学学报,2010,30(4):735-741.
[15]毕哲,胡勇有,孙健.生物阴极型微生物燃料电池同步降解偶氮染料与产电性能研究[J].环境科学学报,2009,29(8):1635-1642.
[16]刘兵.微生物燃料电池处理含酚及特殊废水的应用研究[D].合肥:合肥工业大学,2009.
[17]陈少华,汪家权,夏雪兰,等.双室微生物燃料电池同时去除废水中的苯酚和硝酸盐[J].环境工程学报,2012,06(3):891-895.
[18]Tang X,Du Z,Li H.Anodic electron shuttle mechanism based on1-hydroxy-4-aminoanthraquinone in microbial fuel cells[J].Electrochemistry Communications,2010,12(8):1140-1143.
[19]Guo X,Zhan Y L,Guo S H,et al.Study on start-up and performance of microbial fuel cell with refinery wastewater as fuel[J].Journal of Chemical Engineering of Chinese Universities,2013,27(1):159-163.
[20]国家环境保护总局《水和废水监测分析方法》编委会.水和废水监测分析方法[M].4版.北京:中国环境科学出版社,2002.
[21]Liang Z,Su L I,Guo W,et al.The kinetics for electrochemical removal of ammonia in coking wastewater[J].Chinese Journal of Chemical Engineering,2011,19(4):570-574.
[22]张玉秀,尹莉,李海波,等.焦化废水处理厂活性污泥对硫氰化物的降解机制[J].环境化学,2016,35(1):118-124.
[23]Feng Y,Yi A,Li H,et al.Ocean bacteria:performance on CODCr and NH4(+)-N removal in landfill leachate treatment[J].Water Science&Technology A Journal of the International Association on Water Pollution Research,2015,71(6):817-22.
[24]Pan X,Li Y,Huang H,et al.Biodegradation of thiocyanate and inhibitory interaction with phenol,ammonia in coking wastewater[J].Journal of the Chemical Industry&Engineering Society of China,2009,60(12):3089-3096.
[25]Qi Y,Zhu J,Sun Y,et al.Theoretical Studies of the Binding-affinity and Reactivity Between Laccase and Phenolic Substrates[J].Chemical Journal of Chinese Universities,2014,35(4):776-783.
[26]Luo Y,Zhang R,Liu G,et al.Electricity generation from indole and microbial community analysis in the microbial fuel cell[J].Journal of Hazardous Materials,2010,176(1):759-764.
[27]Gao C Y,Wang A J,Wu W M,et al.Enrichment of anodic biofilm inoculated with anaerobic or aerobic sludge in single chambered aircathode microbial fuel cells.[J].Bioresource Technology,2014,167(3):124-132.
[28]Nair I C,Shashidhar S,microbial degradation of phenol by a species of Alcaligenes isolated from a tropical soil.Soil science.2004,3(4):47-51.
[29]Ma Q,Qu Y Y,Zhang X W,et al.Identification of the microbial community composition and structure of coal-mine wastewater treatment plants[J].Microbiological Research,2015,175:1-5.
[2]杨平,王彬,石炎福,等.生物流化床A-A-O工艺处理焦化废水中试研究[J].化工学报,2002,10(53):1085-1088.
[3]林琳,李玉平,曹宏斌,等.焦化废水厌氧氨氧化生物脱氮的研究[J].中国环境科学,2010,30(9):1201-1206.
[4]张伟,韦朝海,彭平安,等.A/O/O生物流化床处理焦化废水中酚类组成及降解特性分析[J].环境工程学报,2010,2(4):253-257.
[5]徐庆荣,包胜,蔡建安.厌氧/好氧/缺氧(A/O/A)工艺处理焦化废水的试验研究[J].净水技术,2011,30(1):39-41.
[6]Shi S,Qu Y,Ma Q,et al.Performance and microbial community dynamics in bioaugmented aerated filter reactor treating with coking wastewater[J].Bioresource Technology,2015,190:159-166.
[7]柏耀辉,孙庆华,赵翠,等.焦化废水处理系统中喹啉降解菌的种群特征[J].中国环境科学,2008,28(5):449-455.
[8]蒙小俊,李海波,盛宇星,等.焦化废水活性污泥PAH双加氧酶基因多样性分析[J].中国环境科学,2017,37(1):367-372.
[9]唐海,徐建平,安东,等.TiO2/ZSM-5m光催化耦合过硫酸盐降解焦化尾水的研究[J].中国环境科学,2015,35(11):3325-3332.
[10]Kent T D,S.C.Williams BSc MIChemE,Fitzpatrick C S B.Ammoniacal Nitrogen Removal in Biological Aerated Filters:The Effect of Media Size[J].Water&Environment Journal,2010,14(6):409-414.
[11]Qiu Y L,Hanada S,Ohashi A,et al.Syntrophorhabdus aromaticivorans gen.nov.sp.nov.the first cultured anaerobe capable of degrading phenol to acetate in obligate syntrophic associations with a hydrogenotrophic methanogen[J].Applied&Environmental Microbiology,2008,74(7):2051.
[12]郭楚玲,郑天凌.多环芳烃的微生物降解与生物修复[J].海洋环境科学,2000,19(3):24-29.
[13]吴黄英,周培疆,黄强盛.以木质纤维素生物质为降解底物的微生物燃料电池[J].武汉大学学报(理学版),2016,4(32):307-312.
[14]汪家权,夏雪兰,丁巍巍.微生物燃料电池处理苯酚废水运行条件研究[J].环境科学学报,2010,30(4):735-741.
[15]毕哲,胡勇有,孙健.生物阴极型微生物燃料电池同步降解偶氮染料与产电性能研究[J].环境科学学报,2009,29(8):1635-1642.
[16]刘兵.微生物燃料电池处理含酚及特殊废水的应用研究[D].合肥:合肥工业大学,2009.
[17]陈少华,汪家权,夏雪兰,等.双室微生物燃料电池同时去除废水中的苯酚和硝酸盐[J].环境工程学报,2012,06(3):891-895.
[18]Tang X,Du Z,Li H.Anodic electron shuttle mechanism based on1-hydroxy-4-aminoanthraquinone in microbial fuel cells[J].Electrochemistry Communications,2010,12(8):1140-1143.
[19]Guo X,Zhan Y L,Guo S H,et al.Study on start-up and performance of microbial fuel cell with refinery wastewater as fuel[J].Journal of Chemical Engineering of Chinese Universities,2013,27(1):159-163.
[20]国家环境保护总局《水和废水监测分析方法》编委会.水和废水监测分析方法[M].4版.北京:中国环境科学出版社,2002.
[21]Liang Z,Su L I,Guo W,et al.The kinetics for electrochemical removal of ammonia in coking wastewater[J].Chinese Journal of Chemical Engineering,2011,19(4):570-574.
[22]张玉秀,尹莉,李海波,等.焦化废水处理厂活性污泥对硫氰化物的降解机制[J].环境化学,2016,35(1):118-124.
[23]Feng Y,Yi A,Li H,et al.Ocean bacteria:performance on CODCr and NH4(+)-N removal in landfill leachate treatment[J].Water Science&Technology A Journal of the International Association on Water Pollution Research,2015,71(6):817-22.
[24]Pan X,Li Y,Huang H,et al.Biodegradation of thiocyanate and inhibitory interaction with phenol,ammonia in coking wastewater[J].Journal of the Chemical Industry&Engineering Society of China,2009,60(12):3089-3096.
[25]Qi Y,Zhu J,Sun Y,et al.Theoretical Studies of the Binding-affinity and Reactivity Between Laccase and Phenolic Substrates[J].Chemical Journal of Chinese Universities,2014,35(4):776-783.
[26]Luo Y,Zhang R,Liu G,et al.Electricity generation from indole and microbial community analysis in the microbial fuel cell[J].Journal of Hazardous Materials,2010,176(1):759-764.
[27]Gao C Y,Wang A J,Wu W M,et al.Enrichment of anodic biofilm inoculated with anaerobic or aerobic sludge in single chambered aircathode microbial fuel cells.[J].Bioresource Technology,2014,167(3):124-132.
[28]Nair I C,Shashidhar S,microbial degradation of phenol by a species of Alcaligenes isolated from a tropical soil.Soil science.2004,3(4):47-51.
[29]Ma Q,Qu Y Y,Zhang X W,et al.Identification of the microbial community composition and structure of coal-mine wastewater treatment plants[J].Microbiological Research,2015,175:1-5.