废水中硝酸盐的硫自养反硝化工艺处理研究与进展
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摘要
含氮化肥的大量使用和生活、工业等废水的排放与不当处理会造成水体中硝酸盐浓度急剧上升,引起水体富营养化等环境问题,甚至危害人体健康。文中介绍了硫自养反硝化工艺在去除废水中硝酸盐方面的研究与应用,包括分析工艺优缺点、针对工艺缺陷提出解决方案,并阐述了硫自养反硝化工艺与其他工艺相结合的研究进展。同时结合硫铁矿在含水层中生物修复硝酸盐的成功案例,综述了硫铁矿作为反硝化电子供体处理污染水体中硝酸盐的可能性以及处理过程中存在的问题和今后发展。未来硫铁矿作为填料的湿地系统进行反硝化脱氮是可行的。
Excessive use of nitrogenous fertilizers in agricultural activities and inappropriate treatment and emissions of waste waters result in a tremendous increase in the nitrate concentration,and causing eutrophication and other environmental problems for both surface water and groundwater ecosystems and even causing risk to human health.The paper presents a compilation of various autotrophic ways of sulfur denitrification,addresses their advantages and drawbacks,put forward the solutions towards the factors of adverse impact on the wastewater and analyses the research progress of sulfur and sulfide autotrophic denitrification technologies combined with various reactors and other processes.Meanwhile,the paper explores the possibility of pyrite as electron donor in nitrate treatment combined with its successful cases of nitrate bioremediation in the aquifer and discusses the existing problems and future development.Pyrite,as a novel filter material inside the wetland system,is feasible in the nitrogen removal by denitrification in the future.
Excessive use of nitrogenous fertilizers in agricultural activities and inappropriate treatment and emissions of waste waters result in a tremendous increase in the nitrate concentration,and causing eutrophication and other environmental problems for both surface water and groundwater ecosystems and even causing risk to human health.The paper presents a compilation of various autotrophic ways of sulfur denitrification,addresses their advantages and drawbacks,put forward the solutions towards the factors of adverse impact on the wastewater and analyses the research progress of sulfur and sulfide autotrophic denitrification technologies combined with various reactors and other processes.Meanwhile,the paper explores the possibility of pyrite as electron donor in nitrate treatment combined with its successful cases of nitrate bioremediation in the aquifer and discusses the existing problems and future development.Pyrite,as a novel filter material inside the wetland system,is feasible in the nitrogen removal by denitrification in the future.
引文
[1]Zhou W,Sun Y,Wu B,et al.Autotrophic denitrification for nitrate and nitrite removal using sulphur-limestone[J].Journal of Environment Science,2011,23(11):1761-1769.
[2]Zhang W L,Tian Z X,Zhang N,et al.Nitrate pollution of groundwater in northern China[J].Agriculture,Ecosystems&Environment,1996,59(3):223-231.
[3]Wan D,Liu H,Qu J,et al.Using the combined bioelectrochemical and sulfur autotrophic denitrification system for groundwater denitrification[J].Bioresource Technology,2009,100(1):142-148.
[4]Li P,Zuo J,Xing W,et al.Stareh/polyvinyl alcohol blended materials used as solid carbon source for tertiary denitrification of secondary effluent[J],Journal of Environmental Science,2013,25(10):1972-1979.
[5]Rivett M O,Buss S R,Morgan P,et al.Nitrate attenuation in groundwater;A review of biogeochemical controlling processes[J].Water Research,2008,42(16):4215-4232.
[6]Lawrence A,Bisogni J,Batchelor B,et al.Autotrophic denitrification using sulfur electron donors(EPA-600/2-78-113)[M].Washington,DC;US Environmental Protection Agency,1978.
[7]袁莹,周伟丽,王晖.不同载体条件的硫自养反硝化脱氮试验[J].净水技术,2012,31(6):54-58,85.
[8]Francesco Di Capua,Stefano Papirio,Piet N L,et al.Chemolithotrophic denitrification in biofilm reactors[J].Chemical Engineering Journal,2015,280(22):643-657.
[9]Haaijer S C M,Lamers L P M,Smolders A J P,et al.Iron sulfide and pyrite as potential electron donors for microbial nitrate reduction in freshwater wetlands[J].Geomicrobiology Journal,2007,24(5),391-401.
[10]Erkan Sahinkaya,Adem Kilic.Heterotrophic and elemental-sulfurbased autotrophic denitrification processes for simultaneous nitrate and Cr(VI)reduction[J].Water Research,2014,50(1):278-286.
[11]J van der Hoek,J Kappelhof,W Hijnen.Biological nitrate removal from ground water by sulphur/limestone denitrification[J].Journal Chemical Technology and Biotechnology,1992,54:197-200.
[12]Jinwook Chung,Khurram Amin,Seungjin Kim,et al.Autotrophic denitrification of nitrate and nitrite using thiosulfate as an electron donor[J].Water Research,2014,58(3):169-178.
[13]Lee D U,Lee I S,Chai Y D,et al.Effects of external carbon source and empty bed contact time on simultaneous heterotrophic and sulfur-utilizing autotrophic denitrification[J].Process Biochemistry,2001,36(12):1215-1224.
[14]Erkan Sahinkaya,Adem Kilic,Bahadir Duygulu.Pilot and full scale applications of sulfur-based autotrophic denitrification process for nitrate removal from activated sludge process effluent[J].Water Research,2014,60(10):210-217.
[15]Weili Zhou,Yejue Sun,Bingtao Wu,et al.Autotrophic denitrification for nitrate and nitrite removal using sulfur-limestone[J].Journal of Environmental Sciences,2011,23(11):1761-1769.
[16]Erkan Sahinkaya,Nesrin Dursun.Use of elemental sulfur and thiosulfate as electron sources for water denitrification[J].Bioprocess Biosystems Engineering,2015,38(3):531-541.
[17]Laura Christianson,Steven Summerfelt.Fluidization velocity assessment of commercially available sulfur particles for use in autotrophic denitrification biofilters[J].Aquacultural Engineering,2014,60(1):1-5.
[18]Laura Christiansona,Christine Lepinea,Scott Tsukudaa,et al.Nitrate removal effectiveness of fluidized sulfur-based autotrophic denitrification biofilters for recirculating aquaculture systems[J].Aquacultural Engineering,2015,68(4):10-18.
[19]Sher Y,Schneider K,Schwermer C U,et al.Sulfide-induced nitrate reduction in the sludge of an anaerobic digester of a zerodischarge recirculating mariculture system[J].Water Research,2008,42(16):4386-4392.
[20]Summerfelt S T.Design and management of conventional fluidizedsandbiofilters[J].Aquaculture Engineering,2006,34(3):275-302.
[21]Erkan Sahinkaya,Adem Yurtsever,(O|¨)zg(u|¨)r Aktas,et al.Sulfurbased autotrophic denitrification of drinking water using a membrane bioreactor[J].Chemical Engineering Journal,2015,268(10):180-186.
[22]Dongjin Wan,Huijuan Liu,Ruiping Liu,et al.Study of a combined sulfur autotrophic with proton-exchange membrane electrodialytic denitrification technology:Sulfate control and pH balance[J].Bioresource Technology,2011,102(23):10803-10809.
[23]Li Haibo,Zhou Beihai,Tian Zhiyong.Efficient biological nitrogen removal by johannesburg-sulfur autotrophic denitrification from low COD/TN ratio municipal wastewater at low temperature[J].Environmental Earth Sciences,2015,73(9):5027-5035.
[24]Park J H,Kim S H,Ronald D,et al.Enhancement of nitrate removal in constructed wetlands utilizing a combined autotrophic and heterotrophic denitrification technology for treating hydroponic wastewater containing high nitrate and low organic carbon concentrations[J].Agricultural Water Management,2015,162(12):1-14.
[25]Kleerebezem R,Mendez R.Autotrophic denitrification for combined hydrogen sulfide removal from biogas and postdenitrification[J].Water Science Technology,2002,45(1):349-356.
[26]Sahinkaya E,Kilic A,Calimlioglu B,et al.Simultaneous bioreduction of nitrate and chromate using sulfur-based mixotrophic denitrification process[J].Journal of Hazardous Materials,2013,262(22):234-239.
[27]Demirel S,Bayhan I.Nitrate and bromate removal by autotrophic and heterotrophic denitrification processes;Batch experiments[J].Journal of Environmental Health Science Engineering,2013,11(1):1-8.
[28]Luna Velasco A,Sierra Alvarez R,Castro B.Removal of nitrate and hexavalent uranium from groundwater by sequential treatment in bioreactors packed with elemental sulfur and zerovalent iron[J].Biotechnology Bioengineering,2010,107(6):933-942.
[29]Boles A R,Conneely T,McKeever R.Performance of a pilot-scale packed bed bioreactor for perchlorate reduction using a sulfur oxidizing bacterial consortium[J],Biotechnology Bioengineering,2012,109(3):637-646.
[30]Zouboulis A I,Kydros K A,Maris K A.Arsenic(ⅢandⅤ)removal from solutions by pyrite fines[J].Seperation Science Technology,1993,28(15-16):2449-2463.
[31]G(u|¨)lay Bulut,(U|¨)nzile Yenial,Emrecan Emiroglu,et al.Arsenic removal from aqueous solution using pyrite[J].Journal of Cleaner Production,2014,84(1):526-532.
[32]Liu Yuanyuan,Mou Haiyan,Chen Liqun,et al.Cr(Ⅵ)-contaminated groundwater remediation with simulated permeable reactive barrier(PRB)filled with natural pyrite as reactive material:Environmental factors and effectiveness[J].Journal of Hazardous Materials,2015,298(5):83-90.
[33]Jorgensen C J,Jacobsen 0 S,Elberling B,et al.Microbial oxidation of pyrite coupled to nitrate reduction in anoxic groundwater sediment[J].Environmental Science Technology,2009,43(13):4851-4857.
[34]Marc Schwientek,Florian Einsiedl,Willibald Stichler,et al.Evidence for denitrification regulated by pyrite oxidation in a heterogeneous porous groundwater system[J].Chemical Geology,2008,255(1):60-67.
[35]Clara Torrentó,Jordi Unneneta,Neus Otero,et al.Enhanced denitrification in groundwater and sediments from a nitratecontaminated aquifer after addition of pyrite[J].Chemical Geology,2011,287(1-2):90-101.
[36]Clara Torrentó,Jordi Cama,Jordi Unneneta,et al.Denitrification of groundwater with pyrite and Thiobacillus denitrificans[J].Chemical Geology,2010,278(1-2):80-91.
[37]Kong Zhe,Li Lu,Feng Chuanping,et al.Soil infiltration bioreactor incorporated with pyrite-based(mixotrophic)denitrification for domestic wastewater treatment[J].Bioresource Technology,2015,187(13):14-22.
[38]Appelo C A J,Postma D.Geochemistry,groundwater and pollution[J].2nd edition.New York:CRC Press,2005:649.
[39]唐克旺,吴玉成,侯杰.中国地下水资源质量评价(Ⅱ)——地下水水质现状和污染分析[J].水资源保护,2006,22(3):1-4,8.
[2]Zhang W L,Tian Z X,Zhang N,et al.Nitrate pollution of groundwater in northern China[J].Agriculture,Ecosystems&Environment,1996,59(3):223-231.
[3]Wan D,Liu H,Qu J,et al.Using the combined bioelectrochemical and sulfur autotrophic denitrification system for groundwater denitrification[J].Bioresource Technology,2009,100(1):142-148.
[4]Li P,Zuo J,Xing W,et al.Stareh/polyvinyl alcohol blended materials used as solid carbon source for tertiary denitrification of secondary effluent[J],Journal of Environmental Science,2013,25(10):1972-1979.
[5]Rivett M O,Buss S R,Morgan P,et al.Nitrate attenuation in groundwater;A review of biogeochemical controlling processes[J].Water Research,2008,42(16):4215-4232.
[6]Lawrence A,Bisogni J,Batchelor B,et al.Autotrophic denitrification using sulfur electron donors(EPA-600/2-78-113)[M].Washington,DC;US Environmental Protection Agency,1978.
[7]袁莹,周伟丽,王晖.不同载体条件的硫自养反硝化脱氮试验[J].净水技术,2012,31(6):54-58,85.
[8]Francesco Di Capua,Stefano Papirio,Piet N L,et al.Chemolithotrophic denitrification in biofilm reactors[J].Chemical Engineering Journal,2015,280(22):643-657.
[9]Haaijer S C M,Lamers L P M,Smolders A J P,et al.Iron sulfide and pyrite as potential electron donors for microbial nitrate reduction in freshwater wetlands[J].Geomicrobiology Journal,2007,24(5),391-401.
[10]Erkan Sahinkaya,Adem Kilic.Heterotrophic and elemental-sulfurbased autotrophic denitrification processes for simultaneous nitrate and Cr(VI)reduction[J].Water Research,2014,50(1):278-286.
[11]J van der Hoek,J Kappelhof,W Hijnen.Biological nitrate removal from ground water by sulphur/limestone denitrification[J].Journal Chemical Technology and Biotechnology,1992,54:197-200.
[12]Jinwook Chung,Khurram Amin,Seungjin Kim,et al.Autotrophic denitrification of nitrate and nitrite using thiosulfate as an electron donor[J].Water Research,2014,58(3):169-178.
[13]Lee D U,Lee I S,Chai Y D,et al.Effects of external carbon source and empty bed contact time on simultaneous heterotrophic and sulfur-utilizing autotrophic denitrification[J].Process Biochemistry,2001,36(12):1215-1224.
[14]Erkan Sahinkaya,Adem Kilic,Bahadir Duygulu.Pilot and full scale applications of sulfur-based autotrophic denitrification process for nitrate removal from activated sludge process effluent[J].Water Research,2014,60(10):210-217.
[15]Weili Zhou,Yejue Sun,Bingtao Wu,et al.Autotrophic denitrification for nitrate and nitrite removal using sulfur-limestone[J].Journal of Environmental Sciences,2011,23(11):1761-1769.
[16]Erkan Sahinkaya,Nesrin Dursun.Use of elemental sulfur and thiosulfate as electron sources for water denitrification[J].Bioprocess Biosystems Engineering,2015,38(3):531-541.
[17]Laura Christianson,Steven Summerfelt.Fluidization velocity assessment of commercially available sulfur particles for use in autotrophic denitrification biofilters[J].Aquacultural Engineering,2014,60(1):1-5.
[18]Laura Christiansona,Christine Lepinea,Scott Tsukudaa,et al.Nitrate removal effectiveness of fluidized sulfur-based autotrophic denitrification biofilters for recirculating aquaculture systems[J].Aquacultural Engineering,2015,68(4):10-18.
[19]Sher Y,Schneider K,Schwermer C U,et al.Sulfide-induced nitrate reduction in the sludge of an anaerobic digester of a zerodischarge recirculating mariculture system[J].Water Research,2008,42(16):4386-4392.
[20]Summerfelt S T.Design and management of conventional fluidizedsandbiofilters[J].Aquaculture Engineering,2006,34(3):275-302.
[21]Erkan Sahinkaya,Adem Yurtsever,(O|¨)zg(u|¨)r Aktas,et al.Sulfurbased autotrophic denitrification of drinking water using a membrane bioreactor[J].Chemical Engineering Journal,2015,268(10):180-186.
[22]Dongjin Wan,Huijuan Liu,Ruiping Liu,et al.Study of a combined sulfur autotrophic with proton-exchange membrane electrodialytic denitrification technology:Sulfate control and pH balance[J].Bioresource Technology,2011,102(23):10803-10809.
[23]Li Haibo,Zhou Beihai,Tian Zhiyong.Efficient biological nitrogen removal by johannesburg-sulfur autotrophic denitrification from low COD/TN ratio municipal wastewater at low temperature[J].Environmental Earth Sciences,2015,73(9):5027-5035.
[24]Park J H,Kim S H,Ronald D,et al.Enhancement of nitrate removal in constructed wetlands utilizing a combined autotrophic and heterotrophic denitrification technology for treating hydroponic wastewater containing high nitrate and low organic carbon concentrations[J].Agricultural Water Management,2015,162(12):1-14.
[25]Kleerebezem R,Mendez R.Autotrophic denitrification for combined hydrogen sulfide removal from biogas and postdenitrification[J].Water Science Technology,2002,45(1):349-356.
[26]Sahinkaya E,Kilic A,Calimlioglu B,et al.Simultaneous bioreduction of nitrate and chromate using sulfur-based mixotrophic denitrification process[J].Journal of Hazardous Materials,2013,262(22):234-239.
[27]Demirel S,Bayhan I.Nitrate and bromate removal by autotrophic and heterotrophic denitrification processes;Batch experiments[J].Journal of Environmental Health Science Engineering,2013,11(1):1-8.
[28]Luna Velasco A,Sierra Alvarez R,Castro B.Removal of nitrate and hexavalent uranium from groundwater by sequential treatment in bioreactors packed with elemental sulfur and zerovalent iron[J].Biotechnology Bioengineering,2010,107(6):933-942.
[29]Boles A R,Conneely T,McKeever R.Performance of a pilot-scale packed bed bioreactor for perchlorate reduction using a sulfur oxidizing bacterial consortium[J],Biotechnology Bioengineering,2012,109(3):637-646.
[30]Zouboulis A I,Kydros K A,Maris K A.Arsenic(ⅢandⅤ)removal from solutions by pyrite fines[J].Seperation Science Technology,1993,28(15-16):2449-2463.
[31]G(u|¨)lay Bulut,(U|¨)nzile Yenial,Emrecan Emiroglu,et al.Arsenic removal from aqueous solution using pyrite[J].Journal of Cleaner Production,2014,84(1):526-532.
[32]Liu Yuanyuan,Mou Haiyan,Chen Liqun,et al.Cr(Ⅵ)-contaminated groundwater remediation with simulated permeable reactive barrier(PRB)filled with natural pyrite as reactive material:Environmental factors and effectiveness[J].Journal of Hazardous Materials,2015,298(5):83-90.
[33]Jorgensen C J,Jacobsen 0 S,Elberling B,et al.Microbial oxidation of pyrite coupled to nitrate reduction in anoxic groundwater sediment[J].Environmental Science Technology,2009,43(13):4851-4857.
[34]Marc Schwientek,Florian Einsiedl,Willibald Stichler,et al.Evidence for denitrification regulated by pyrite oxidation in a heterogeneous porous groundwater system[J].Chemical Geology,2008,255(1):60-67.
[35]Clara Torrentó,Jordi Unneneta,Neus Otero,et al.Enhanced denitrification in groundwater and sediments from a nitratecontaminated aquifer after addition of pyrite[J].Chemical Geology,2011,287(1-2):90-101.
[36]Clara Torrentó,Jordi Cama,Jordi Unneneta,et al.Denitrification of groundwater with pyrite and Thiobacillus denitrificans[J].Chemical Geology,2010,278(1-2):80-91.
[37]Kong Zhe,Li Lu,Feng Chuanping,et al.Soil infiltration bioreactor incorporated with pyrite-based(mixotrophic)denitrification for domestic wastewater treatment[J].Bioresource Technology,2015,187(13):14-22.
[38]Appelo C A J,Postma D.Geochemistry,groundwater and pollution[J].2nd edition.New York:CRC Press,2005:649.
[39]唐克旺,吴玉成,侯杰.中国地下水资源质量评价(Ⅱ)——地下水水质现状和污染分析[J].水资源保护,2006,22(3):1-4,8.
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