三维生物膜电极反应器去除地下水中硝酸氮
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摘要
采用三维生物膜电极反应器(three-dimensional biofilm electrode reactor,3D-BER)并接种氢自养反硝化菌,研究了不同因素对其处理地下水中硝酸氮的影响。结果表明:反应器的电极间距减小有利于硝酸氮的去除,但会增加亚硝酸氮积累的风险,适宜的极板间距为50 mm;去除硝酸氮的最佳电流强度范围为40~60 mA,最适进水硝酸氮浓度范围为35~50 mg·L~(-1),最佳进水pH的范围为7.5~8.5,最佳水力停留时间为12 h。该条件下反应器运行效果稳定,不需外加氢源和碳源。通过与不接种氢自养反硝化菌的反应器进行对比分析,认为随着电流强度的增加,纯电化学作用对硝酸氮的还原作用也增强,但纯电化学反应在反应器脱氮过程中的比例远小于生物作用。3D-BER对硝酸氮的去除是由氢自养反硝化作用、电化学反应与部分异养反硝化共同作用的结果。
Main factors influencing the removal effect of nitrate nitrogen from groundwater were studied using three dimensional biofilm electrode reactor(3D-BER)inoculated with autohydrogenotrophic denitrification bacteria. The results showed that the reduction of space between electrodes is benifit to the removal of nitrate nitrogen whereas the nitrite nitrogen accumulation will increase, and the appropriate space is 50 mm. The optimum condition removing nitrate from the reactor are from 40 to 60 mA of current intensity, 35 to 50 mg·L~(-1) NO_3-N in influent, pH 7.5 to 8.5 and HRT no less than 12 h, under which no more hydrogen and carbon are needed with the reactor running stably. In order to understand the mechanism of 3D-BER, two reactors with or without autohydrogenotrophic denitrification bacteria were compared. The results showed that that electrochemical reduction action of NO_3-N increase with the augment of current intensity, but the pure electrochemical reaction accounts for less percentage in the removal of nitrate in 3D-BER compared to biological denitrification action. The removal of NO_3-N in 3D-BER is combined effects by electrochemical reaction, autohydrogenotrophic bacteria denitrification and partial heterotrophic denitrification.
Main factors influencing the removal effect of nitrate nitrogen from groundwater were studied using three dimensional biofilm electrode reactor(3D-BER)inoculated with autohydrogenotrophic denitrification bacteria. The results showed that the reduction of space between electrodes is benifit to the removal of nitrate nitrogen whereas the nitrite nitrogen accumulation will increase, and the appropriate space is 50 mm. The optimum condition removing nitrate from the reactor are from 40 to 60 mA of current intensity, 35 to 50 mg·L~(-1) NO_3-N in influent, pH 7.5 to 8.5 and HRT no less than 12 h, under which no more hydrogen and carbon are needed with the reactor running stably. In order to understand the mechanism of 3D-BER, two reactors with or without autohydrogenotrophic denitrification bacteria were compared. The results showed that that electrochemical reduction action of NO_3-N increase with the augment of current intensity, but the pure electrochemical reaction accounts for less percentage in the removal of nitrate in 3D-BER compared to biological denitrification action. The removal of NO_3-N in 3D-BER is combined effects by electrochemical reaction, autohydrogenotrophic bacteria denitrification and partial heterotrophic denitrification.
引文
[1]MICHAEL O R,STEPHEN R B,PHILIP M,et al.Nitrate attenuation in groundwater:A review of biogeochemical controlling processes[J].Water Research,2008,42(7):4215-4232.DOI:10.1016/j.watres.2008.07.020.
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[4]ZHOU M H,FU W J,GU H Y,et al.Nitrate removal from groundwater by a novel three-dimensional electrode biofilm reactor[J].Electrochimica Acta,2007,52(3):6052-6058.DOI:10.1016/j.electacta.2007.03.064.
[5]陈建平.三维电极生物膜反应器脱除低C/N值废水中硝酸盐氮和COD[D].武汉:华中科技大学,2006.
[6]马生军.新型三维电极生物膜工艺强化脱氮除磷特性[J].水处理技术,2016,42(4):39-41.
[7]国家环境保护总局.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.
[8]GHAFARI S,HASAN M,AROUA M K.Nitrate remediation in a novel upflow bio-electrochemical reactor(UBER)using palm shell activated carbon as cathode material[J].Electrochimica Acta,2009,54(17):4164-4171.DOI:10.1016/j.electacta.2009.02.062.
[9]SAKAKIBARA Y,NAKAYAMA T.A novel multi-electrode system for electrolytic and biological water treatments:electric charge transfer and application to denitrification[J].Water Research,2001,35(3):768-778.DOI:10.1016/S0043-1354(00)00327-4.
[10]周欲飞.电极生物膜组合工艺去除地下水硝酸盐的试验研究[D].杭州:浙江大学,2010.
[11]葛艳菊.电极-生物膜反应器去除厌氧氨氧化出水中硝酸盐的性能研究[D].北京:北京市环境保护科学研究院,2007.
[12]赵国智.电极生物膜反硝化去除地下水中硝酸盐氮的实验研究[D].杭州:浙江大学,2011.
[13]郭劲松,杨琳,陈猷鹏,等.三维电极生物膜反应器全程自养脱氮的启动研究[J].环境科学学报,2012,32(6):1342-1347.
[14]冯玉杰,李晓岩.电化学技术在环境工程中的应用[M].北京:化学工业出版社,2002:24-25.
[15]XING X,SCHERSON D A,MAK C.Electrocatalitic reduction of nitrate mediated by underpotential-deposited cadmium on gold and silver electrodes in acid media[J].Journal of the Electrochemical Society,1990,137:2166-2172.DOI:10.1149/1.2086905.
[16]范经华,范彬,鹿道强,等.多孔钛板负载Pd-Cu阴极电催化还原饮用水中硝酸盐的研究[J].环境科学,2006,27(6):1117-1122.
[17]郝瑞霞,任晓克,孟成成,等.ρ(C)/ρ(N)对3BER-S工艺特性及反硝化细菌群落特征的影响[J].北京工业大学学报,2015,41(5):755-762.
[18]ROBERT B M,JORG R,WILBUR H,et al.Reduction of nitrate and nitrite in water by immobilized enzymes[J].Nature,1992,355(20):717-719.DOI:10.1038/355717a0.
[19]SHAHIN G,MOHAMED K A,MASITAH H.Control of p H during water denitrification in an upflow bio-electrochemical reactor(UBER)using a pump around system[J].Separation and Purification Technology,2010,72(3):401-405.DOI:10.1016/j.seppur.2010.03.014.
[20]MICHAL P,YUTAKA S,MASAO K.High-rate denitrification and SS rejection by biofilm-electrode reactor(BER)combined with microfiltration[J].Water Research,2002,36(19):4801-4810.DOI:10.1016/S0043-1354(02)00206-3.
[2]FELEKE Z,ARAKI K,SAKAKIBARA Y,et al.Selective reduction of nitrate to nitrogen gas in a biofilm-electrode reactor[J].Water Research,1998,32(9):2728-2734.DOI:10.1016/S0043-1354(98)00018-9.
[3]MATTEO D,MARC T M.Powering denitrification:The perspectives of electrocatalytic nitrate reduction[J].Energy&Environmental Science,2012,5(12):9726-9742.DOI:10.1039/C2EE23062C.
[4]ZHOU M H,FU W J,GU H Y,et al.Nitrate removal from groundwater by a novel three-dimensional electrode biofilm reactor[J].Electrochimica Acta,2007,52(3):6052-6058.DOI:10.1016/j.electacta.2007.03.064.
[5]陈建平.三维电极生物膜反应器脱除低C/N值废水中硝酸盐氮和COD[D].武汉:华中科技大学,2006.
[6]马生军.新型三维电极生物膜工艺强化脱氮除磷特性[J].水处理技术,2016,42(4):39-41.
[7]国家环境保护总局.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.
[8]GHAFARI S,HASAN M,AROUA M K.Nitrate remediation in a novel upflow bio-electrochemical reactor(UBER)using palm shell activated carbon as cathode material[J].Electrochimica Acta,2009,54(17):4164-4171.DOI:10.1016/j.electacta.2009.02.062.
[9]SAKAKIBARA Y,NAKAYAMA T.A novel multi-electrode system for electrolytic and biological water treatments:electric charge transfer and application to denitrification[J].Water Research,2001,35(3):768-778.DOI:10.1016/S0043-1354(00)00327-4.
[10]周欲飞.电极生物膜组合工艺去除地下水硝酸盐的试验研究[D].杭州:浙江大学,2010.
[11]葛艳菊.电极-生物膜反应器去除厌氧氨氧化出水中硝酸盐的性能研究[D].北京:北京市环境保护科学研究院,2007.
[12]赵国智.电极生物膜反硝化去除地下水中硝酸盐氮的实验研究[D].杭州:浙江大学,2011.
[13]郭劲松,杨琳,陈猷鹏,等.三维电极生物膜反应器全程自养脱氮的启动研究[J].环境科学学报,2012,32(6):1342-1347.
[14]冯玉杰,李晓岩.电化学技术在环境工程中的应用[M].北京:化学工业出版社,2002:24-25.
[15]XING X,SCHERSON D A,MAK C.Electrocatalitic reduction of nitrate mediated by underpotential-deposited cadmium on gold and silver electrodes in acid media[J].Journal of the Electrochemical Society,1990,137:2166-2172.DOI:10.1149/1.2086905.
[16]范经华,范彬,鹿道强,等.多孔钛板负载Pd-Cu阴极电催化还原饮用水中硝酸盐的研究[J].环境科学,2006,27(6):1117-1122.
[17]郝瑞霞,任晓克,孟成成,等.ρ(C)/ρ(N)对3BER-S工艺特性及反硝化细菌群落特征的影响[J].北京工业大学学报,2015,41(5):755-762.
[18]ROBERT B M,JORG R,WILBUR H,et al.Reduction of nitrate and nitrite in water by immobilized enzymes[J].Nature,1992,355(20):717-719.DOI:10.1038/355717a0.
[19]SHAHIN G,MOHAMED K A,MASITAH H.Control of p H during water denitrification in an upflow bio-electrochemical reactor(UBER)using a pump around system[J].Separation and Purification Technology,2010,72(3):401-405.DOI:10.1016/j.seppur.2010.03.014.
[20]MICHAL P,YUTAKA S,MASAO K.High-rate denitrification and SS rejection by biofilm-electrode reactor(BER)combined with microfiltration[J].Water Research,2002,36(19):4801-4810.DOI:10.1016/S0043-1354(02)00206-3.