N-亚硝胺在不同处理工艺污水处理厂中的分布及其去除
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摘要
以6种典型N-亚硝胺(NAs)为研究对象,基于质量浓度监测数据系统研究了它们在3种不同处理工艺的污水处理厂中的分布及其去除规律,并分析了它们在受纳河水中的污染概况及来源.结果表明,6种NAs在3种不同处理工艺污水处理厂各工艺段废水中普遍存在,其中主要污染物为NPIP、NDMA和NPYR,质量浓度水平为几十到几百ng·L-1. 3种不同处理工艺的污水处理厂都能对NAs起到一定的去除效果,其中改良A~2/O和A~2/O+MBR对NAs的去除效果较好,总体去除率分别为95%和63%,主要依靠生化阶段的微生物降解和转化.在过滤、MBR和消毒阶段,废水处理体系中NAs前驱物经一系列反应后会形成一定的NAs增量. 6种NAs在受纳河流的表层水中也频繁检出,主要污染物和污水处理厂进水中的主要污染物一致,仍然是MDMA、NPIP和NPYR.受纳河流中的NAs来源广泛而复杂,包括污水处理厂尾水排入、未经处理的生活污水和工业废水以及工业区地表径流等的汇入.因此,应该通过增强污水收集和处理能力、优化污水处理工艺等措施减少NAs向受纳河流的输入.
This study measured the concentrations of six N-nitrosamines( NAs) in water samples from each process stage of three wastewater treatment plants( WWTPs) and their corresponding receiving rivers. The occurrence and removal of NAs was then systematically studied in three WWTPs using different treatment processes,and their pollution profiles and sources in the receiving rivers were analyzed. The results showed that the six NAs occurred widely in the wastewater from every process stage of three WWTPs.NPIP,NDMA,and NPYR were the dominant pollutants with concentrations in the tens to hundreds ng·L-1. The three WWTPs using different treatment processes removed a certain amount of NAs,and the modified A2/O and A2/O + MBR showed good NAs removal effects,with total removal rates of 95% and 63%,respectively. The removal of NAs mainly relied on microbial degradation and transformation during the biochemical stage. During the filtration,disinfection,and MBR stages,NAs precursors in the wastewater treatment system could form some added NAs after a series of reactions. The six NAs were also frequently detected in the surface waters of receiving rivers,where the main pollutants were also MDMA,NPIP,and NPYR,which was consistent with the influent of the WTTPs. The sources of NAs in the receiving rivers were wide ranging and complicated,including emission from the effluent of the WTTPs,the release of untreated sanitary sewage,industrial wastewater,and surface runoff from industrial districts. Therefore,effective measures should be taken to reduce the input of NAs into receiving rivers,such as enhancing the capacity of sewage collection and treatment and optimizing sewage treatment processes.
This study measured the concentrations of six N-nitrosamines( NAs) in water samples from each process stage of three wastewater treatment plants( WWTPs) and their corresponding receiving rivers. The occurrence and removal of NAs was then systematically studied in three WWTPs using different treatment processes,and their pollution profiles and sources in the receiving rivers were analyzed. The results showed that the six NAs occurred widely in the wastewater from every process stage of three WWTPs.NPIP,NDMA,and NPYR were the dominant pollutants with concentrations in the tens to hundreds ng·L-1. The three WWTPs using different treatment processes removed a certain amount of NAs,and the modified A2/O and A2/O + MBR showed good NAs removal effects,with total removal rates of 95% and 63%,respectively. The removal of NAs mainly relied on microbial degradation and transformation during the biochemical stage. During the filtration,disinfection,and MBR stages,NAs precursors in the wastewater treatment system could form some added NAs after a series of reactions. The six NAs were also frequently detected in the surface waters of receiving rivers,where the main pollutants were also MDMA,NPIP,and NPYR,which was consistent with the influent of the WTTPs. The sources of NAs in the receiving rivers were wide ranging and complicated,including emission from the effluent of the WTTPs,the release of untreated sanitary sewage,industrial wastewater,and surface runoff from industrial districts. Therefore,effective measures should be taken to reduce the input of NAs into receiving rivers,such as enhancing the capacity of sewage collection and treatment and optimizing sewage treatment processes.
引文
[1] Planas C,Palaciosó,Ventura F,et al. Analysis of nitrosamines in water by automated SPE and isotope dilution GC/HRMS:occurrence in the different steps of a drinking water treatment plant,and in chlorinated samples from a reservoir and a sewage treatment plant effluent[J]. Talanta,2008,76(4):906-913.
[2] Gushgari A J,Halden R U. Critical review of major sources of human exposure to N-nitrosamines[J]. Chemosphere,2018,210:1124-1136.
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[4] Liao X B,Bei E,Li S X,et al. Applying the polarity rapid assessment method to characterize nitrosamine precursors and to understand their removal by drinking water treatment processes[J]. Water Research,2015,87:292-298.
[5] Krauss M,Longrée P,Dorusch F,et al. Occurrence and removal of N-nitrosamines in wastewater treatment plants[J]. Water Research,2009,43(17):4381-4391.
[6] Ma F J,Wan Y,Yuan G X,et al. Occurrence and source of nitrosamines and secondary amines in groundwater and its adjacent Jialu River basin,China[J]. Environmental Science&Technology,2012,46(6):3236-3243.
[7] Wang W F,Yu J W,An W,et al. Occurrence and profiling of multiple nitrosamines in source water and drinking water of China[J]. Science of the Total Environment,2016,551-552:489-495.
[8] Park J E,Seo J E,Lee J Y,et al. Distribution of seven Nnitrosamines in food[J]. Toxicological Research,2015,31(3):279-288.
[9] Zhao Y Y,Boyd J M,Woodbeck M,et al. Formation of Nnitrosamines from eleven disinfection treatments of seven different surface waters[J]. Environmental Science&Technology,2008,42(13):4857-4862.
[10] Nawrocki J, Andrzejewski P. Nitrosamines and water[J].Journal of Hazardous Materials,2011,189(1-2):1-18.
[11] Sgroi M, Vagliasindi F G A, Snyder S A, et al. NNitrosodimethylamine(NDMA)and its precursors in water and wastewater:a review on formation and removal[J].Chemosphere,2018,191:685-703.
[12] Mitch W A,Sedlak D L. Formation of N-nitrosodimethylamine(NDMA)from dimethylamine during chlorination[J].Environmental Science&Technology,2002,36(4):588-595.
[13] van Huy N,Murakami M,Sakai H,et al. Occurrence and formation potential of N-nitrosodimethylamine in ground water and river water in Tokyo[J]. Water Research,2011,45(11):3369-3377.
[14]余卫军,邱月升,王佩,等.气相色谱-三重四极杆质谱测定广东地区市售腊肠中9种挥发性亚硝胺[J].肉类研究,2016,30(6):29-34.Yu W J,Qiu Y S,Wang P,et al. Investigation of nine volatile nitrosamines in sausages marketed in Guangdong province by gas chromatography tandem triple quadrupole mass spectrometry(GC-MS-MS)[J]. Meat Research,2016,30(6):29-34.
[15] Qiu Y,Chen J H,Yu W,et al. Contamination of Chinese salted fish with volatile N-nitrosamines as determined by QuEChERS and gas chromatography-tandem mass spectrometry[J]. Food Chemistry,2017,232:763-769.
[16]董蕾,王海燕,蔡宏铨,等.我国六城市饮用水中含氮消毒副产物的现状调查[J].环境与健康杂志,2016,33(3):232-235.Dong L,Wang H Y,Cai H Q,et al. Investigation on nitrogenous disinfection by-products in drinking water in six cities,China[J]. Journal of Environment and Health,2016,33(3):232-235.
[17]胡敏,罗正盛.气质联用测定橡胶中的11种N-亚硝胺物质的释放量[J].广州化工,2016,44(14):130-132.Hu M,Luo Z S. Determination of 11 N-nitrosamines release in rubber by GCMS[J]. Guangzhou Chemical Industry,2016,44(14):130-132.
[18]谢永萍,赖红霞,李慧勇,等.橡胶气球中有害物质的风险分析[J].当代化工,2018,47(11):2309-2312.Xie Y P,Lai H X,Li H Y,et al. Risk analysis of harmful substances in the rubber balloon[J]. Contemporary Chemical Industry,2018,47(11):2309-2312.
[19]周超. UV-H2O2降解去除饮用水消毒副产物亚硝胺类的性能研究[J].水处理技术,2015,41(3):48-53.Zhou C. Performance of ultraviolet irradiation/hydrogen peroxide(UV-H2O2)on the degradation of nitrosamines in drinking water[J]. Technology of Water Treatment,2015,41(3):48-53.
[20]黄耀.饮用水处理中亚硝胺类物质的生物降解研究[D].新乡:河南师范大学,2014.Huang Y. Biological degradation of nitrosamines in drinking water treatment[D]. Xinxiang:Henan Normal University,2014.
[21] Wang C,Zhang X,Wang J,et al. Effects of organic fractions on the formation and control of N-nitrosamine precursors during conventional drinking water treatment processes[J]. Science of the Total Environment,2013,449:295-301.
[22]张秋秋,潘申龄,张昱,等.我国城市饮用水中N-亚硝基二甲胺的健康风险评估及水质标准制定[J].环境科学,2017,38(7):2747-2753.Zhang Q Q,Pan S L,Zhang Y,et al. Estimation of health risk and enaction of safety standards of N-nitrosodimethylamine(NDMA)in drinking waters in China[J]. Environmental Science,2017,38(7):2747-2753.
[23] Bei E,Shu Y Y,Li S X,et al. Occurrence of nitrosamines and their precursors in drinking water systems around mainland China[J]. Water Research,2016,98:168-175.
[24] Lee J H,Oh J E. A comprehensive survey on the occurrence and fate of nitrosamines in sewage treatment plants and water environment[J]. Science of the Total Environment,2016,556:330-337.
[25]郑莹,金鹏康,金鑫,等.二级出水中亚硝胺类消毒副产物分布及臭氧化特性[J].环境工程学报,2018,12(3):751-759.Zheng Y,Jin P K,Jin Y,et al. Distribution and ozonation characteristics of nitrosamines in wastewater treatment plant effluent[J]. Chinese Journal of Environmental Engineering,2018,12(3):751-759.
[26] Hu H D,Jiang C,Ma H J,et al. Removal characteristics of DON in pharmaceutical wastewater and its influence on the Nnitrosodimethylamine formation potential and acute toxicity of DOM[J]. Water Research,2017,109:114-121.
[27] Wang L,Li Y M,Shang X L,et al. Occurrence and removal of N-nitrosodimethylamine and its precursors in wastewater treatment plants in and around Shanghai[J]. Frontiers of Environmental Science&Engineering,2014,8(4):519-530.
[28]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.
[29] Boyd J M,Hrudey S E,Li X F,et al. Solid-phase extraction and high-performance liquid chromatography mass spectrometry analysis of nitrosamines in treated drinking water and wastewater[J]. Tr AC Trends in Analytical Chemistry,2011,30(9):1410-1421.
[30] Gerrity D,Pisarenko A N,Marti E,et al. Nitrosamines in pilotscale and full-scale wastewater treatment plants with ozonation[J]. Water Research,2015,72:251-261.
[31] Padhye L,Tezel U,Mitch W A,et al. Occurrence and fate of nitrosamines and their precursors in municipal sludge and anaerobic digestion systems[J]. Environmental Science&Technology,2009,43(9):3087-3093.
[32]姚瑞雄.分散固相萃取-同位素稀释-气相色谱-质谱法测定酱油中5种N-亚硝胺[J].分析试验室,2018,37(2):183-187.Yao R X. Simultaneous determination of five N-nitrosamines in soy sauces by dispersive solid-phase extraction and isotope dilution-gas chromatography-mass spectrometry[J]. Chinese Journal of Analysis Laboratory,2018,37(2):183-187.
[33] Fan C C,Lin T F. N-nitrosamines in drinking water and beer:Detection and risk assessment[J]. Chemosphere,2018,200:48-56.
[34]章若红,徐德佳,江艳,等.与食品接触橡胶制品中N-亚硝胺的来源、危害及控制[J].世界橡胶工业,2011,38(4):33-36.Zhang R H,Xu D J,Jiang Y,et al. Sources,harm and control of N-nitrosamine in rubber products contacted with food[J].World Rubber Industry,2011,38(4):33-36.
[35] Chon K,Kim S H,Cho J. Removal of N-nitrosamines in a membrane bioreactor and nanofiltration hybrid system for municipal wastewater reclamation:process efficiency and mechanisms[J]. Bioresource Technology,2015,190:499-507.
[36] Wijekoon K C,Fujioka T,Mc Donald J A,et al. Removal of Nnitrosamines by an aerobic membrane bioreactor[J]. Bioresource Technology,2013,141:41-45.
[37] Yoon S,Nakada N,Tanaka H. Occurrence and fate of Nnitrosamines and their formation potential in three wastewater treatment plants in Japan[J]. Water Science&Technology,2013,68(10):2118-2126.
[38] Plumlee M H, López-Mesas M, Heidlberger A, et al. Nnitrosodimethylamine(NDMA)removal by reverse osmosis and UV treatment and analysis via LC-MS/MS[J]. Water Research,2008,42(1-2):347-355.
[39] Yoon S,Nakada N,Tanaka H. Occurrence and removal of NDMA and NDMA formation potential in wastewater treatment plants[J]. Journal of Hazardous Materials,2011,190(1-3):897-902.
[40] Zhou W J,Chen C P,Lou L J,et al. Formation potential of nine nitrosamines from corresponding secondary amines by chloramination[J]. Chemosphere,2014,95:81-87.
[41]陈贻龙.地下式MBR工艺在广州京溪污水处理厂的应用[J].给水排水,2010,36(7):51-54.Chen Y L. Application of underground MBR in Guangzhou Jingxi wastewater treatment plant[J]. Water&Wastewater Engineering,2010,36(7):51-54.
[2] Gushgari A J,Halden R U. Critical review of major sources of human exposure to N-nitrosamines[J]. Chemosphere,2018,210:1124-1136.
[3] Richardson S D,Plewa M J,Wagner E D,et al. Occurrence,genotoxicity, and carcinogenicity of regulated and emerging disinfection by-products in drinking water:a review and roadmap for research[J]. Mutation Research/Reviews in Mutation Research,2007,636(1-3):178-242.
[4] Liao X B,Bei E,Li S X,et al. Applying the polarity rapid assessment method to characterize nitrosamine precursors and to understand their removal by drinking water treatment processes[J]. Water Research,2015,87:292-298.
[5] Krauss M,Longrée P,Dorusch F,et al. Occurrence and removal of N-nitrosamines in wastewater treatment plants[J]. Water Research,2009,43(17):4381-4391.
[6] Ma F J,Wan Y,Yuan G X,et al. Occurrence and source of nitrosamines and secondary amines in groundwater and its adjacent Jialu River basin,China[J]. Environmental Science&Technology,2012,46(6):3236-3243.
[7] Wang W F,Yu J W,An W,et al. Occurrence and profiling of multiple nitrosamines in source water and drinking water of China[J]. Science of the Total Environment,2016,551-552:489-495.
[8] Park J E,Seo J E,Lee J Y,et al. Distribution of seven Nnitrosamines in food[J]. Toxicological Research,2015,31(3):279-288.
[9] Zhao Y Y,Boyd J M,Woodbeck M,et al. Formation of Nnitrosamines from eleven disinfection treatments of seven different surface waters[J]. Environmental Science&Technology,2008,42(13):4857-4862.
[10] Nawrocki J, Andrzejewski P. Nitrosamines and water[J].Journal of Hazardous Materials,2011,189(1-2):1-18.
[11] Sgroi M, Vagliasindi F G A, Snyder S A, et al. NNitrosodimethylamine(NDMA)and its precursors in water and wastewater:a review on formation and removal[J].Chemosphere,2018,191:685-703.
[12] Mitch W A,Sedlak D L. Formation of N-nitrosodimethylamine(NDMA)from dimethylamine during chlorination[J].Environmental Science&Technology,2002,36(4):588-595.
[13] van Huy N,Murakami M,Sakai H,et al. Occurrence and formation potential of N-nitrosodimethylamine in ground water and river water in Tokyo[J]. Water Research,2011,45(11):3369-3377.
[14]余卫军,邱月升,王佩,等.气相色谱-三重四极杆质谱测定广东地区市售腊肠中9种挥发性亚硝胺[J].肉类研究,2016,30(6):29-34.Yu W J,Qiu Y S,Wang P,et al. Investigation of nine volatile nitrosamines in sausages marketed in Guangdong province by gas chromatography tandem triple quadrupole mass spectrometry(GC-MS-MS)[J]. Meat Research,2016,30(6):29-34.
[15] Qiu Y,Chen J H,Yu W,et al. Contamination of Chinese salted fish with volatile N-nitrosamines as determined by QuEChERS and gas chromatography-tandem mass spectrometry[J]. Food Chemistry,2017,232:763-769.
[16]董蕾,王海燕,蔡宏铨,等.我国六城市饮用水中含氮消毒副产物的现状调查[J].环境与健康杂志,2016,33(3):232-235.Dong L,Wang H Y,Cai H Q,et al. Investigation on nitrogenous disinfection by-products in drinking water in six cities,China[J]. Journal of Environment and Health,2016,33(3):232-235.
[17]胡敏,罗正盛.气质联用测定橡胶中的11种N-亚硝胺物质的释放量[J].广州化工,2016,44(14):130-132.Hu M,Luo Z S. Determination of 11 N-nitrosamines release in rubber by GCMS[J]. Guangzhou Chemical Industry,2016,44(14):130-132.
[18]谢永萍,赖红霞,李慧勇,等.橡胶气球中有害物质的风险分析[J].当代化工,2018,47(11):2309-2312.Xie Y P,Lai H X,Li H Y,et al. Risk analysis of harmful substances in the rubber balloon[J]. Contemporary Chemical Industry,2018,47(11):2309-2312.
[19]周超. UV-H2O2降解去除饮用水消毒副产物亚硝胺类的性能研究[J].水处理技术,2015,41(3):48-53.Zhou C. Performance of ultraviolet irradiation/hydrogen peroxide(UV-H2O2)on the degradation of nitrosamines in drinking water[J]. Technology of Water Treatment,2015,41(3):48-53.
[20]黄耀.饮用水处理中亚硝胺类物质的生物降解研究[D].新乡:河南师范大学,2014.Huang Y. Biological degradation of nitrosamines in drinking water treatment[D]. Xinxiang:Henan Normal University,2014.
[21] Wang C,Zhang X,Wang J,et al. Effects of organic fractions on the formation and control of N-nitrosamine precursors during conventional drinking water treatment processes[J]. Science of the Total Environment,2013,449:295-301.
[22]张秋秋,潘申龄,张昱,等.我国城市饮用水中N-亚硝基二甲胺的健康风险评估及水质标准制定[J].环境科学,2017,38(7):2747-2753.Zhang Q Q,Pan S L,Zhang Y,et al. Estimation of health risk and enaction of safety standards of N-nitrosodimethylamine(NDMA)in drinking waters in China[J]. Environmental Science,2017,38(7):2747-2753.
[23] Bei E,Shu Y Y,Li S X,et al. Occurrence of nitrosamines and their precursors in drinking water systems around mainland China[J]. Water Research,2016,98:168-175.
[24] Lee J H,Oh J E. A comprehensive survey on the occurrence and fate of nitrosamines in sewage treatment plants and water environment[J]. Science of the Total Environment,2016,556:330-337.
[25]郑莹,金鹏康,金鑫,等.二级出水中亚硝胺类消毒副产物分布及臭氧化特性[J].环境工程学报,2018,12(3):751-759.Zheng Y,Jin P K,Jin Y,et al. Distribution and ozonation characteristics of nitrosamines in wastewater treatment plant effluent[J]. Chinese Journal of Environmental Engineering,2018,12(3):751-759.
[26] Hu H D,Jiang C,Ma H J,et al. Removal characteristics of DON in pharmaceutical wastewater and its influence on the Nnitrosodimethylamine formation potential and acute toxicity of DOM[J]. Water Research,2017,109:114-121.
[27] Wang L,Li Y M,Shang X L,et al. Occurrence and removal of N-nitrosodimethylamine and its precursors in wastewater treatment plants in and around Shanghai[J]. Frontiers of Environmental Science&Engineering,2014,8(4):519-530.
[28]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.
[29] Boyd J M,Hrudey S E,Li X F,et al. Solid-phase extraction and high-performance liquid chromatography mass spectrometry analysis of nitrosamines in treated drinking water and wastewater[J]. Tr AC Trends in Analytical Chemistry,2011,30(9):1410-1421.
[30] Gerrity D,Pisarenko A N,Marti E,et al. Nitrosamines in pilotscale and full-scale wastewater treatment plants with ozonation[J]. Water Research,2015,72:251-261.
[31] Padhye L,Tezel U,Mitch W A,et al. Occurrence and fate of nitrosamines and their precursors in municipal sludge and anaerobic digestion systems[J]. Environmental Science&Technology,2009,43(9):3087-3093.
[32]姚瑞雄.分散固相萃取-同位素稀释-气相色谱-质谱法测定酱油中5种N-亚硝胺[J].分析试验室,2018,37(2):183-187.Yao R X. Simultaneous determination of five N-nitrosamines in soy sauces by dispersive solid-phase extraction and isotope dilution-gas chromatography-mass spectrometry[J]. Chinese Journal of Analysis Laboratory,2018,37(2):183-187.
[33] Fan C C,Lin T F. N-nitrosamines in drinking water and beer:Detection and risk assessment[J]. Chemosphere,2018,200:48-56.
[34]章若红,徐德佳,江艳,等.与食品接触橡胶制品中N-亚硝胺的来源、危害及控制[J].世界橡胶工业,2011,38(4):33-36.Zhang R H,Xu D J,Jiang Y,et al. Sources,harm and control of N-nitrosamine in rubber products contacted with food[J].World Rubber Industry,2011,38(4):33-36.
[35] Chon K,Kim S H,Cho J. Removal of N-nitrosamines in a membrane bioreactor and nanofiltration hybrid system for municipal wastewater reclamation:process efficiency and mechanisms[J]. Bioresource Technology,2015,190:499-507.
[36] Wijekoon K C,Fujioka T,Mc Donald J A,et al. Removal of Nnitrosamines by an aerobic membrane bioreactor[J]. Bioresource Technology,2013,141:41-45.
[37] Yoon S,Nakada N,Tanaka H. Occurrence and fate of Nnitrosamines and their formation potential in three wastewater treatment plants in Japan[J]. Water Science&Technology,2013,68(10):2118-2126.
[38] Plumlee M H, López-Mesas M, Heidlberger A, et al. Nnitrosodimethylamine(NDMA)removal by reverse osmosis and UV treatment and analysis via LC-MS/MS[J]. Water Research,2008,42(1-2):347-355.
[39] Yoon S,Nakada N,Tanaka H. Occurrence and removal of NDMA and NDMA formation potential in wastewater treatment plants[J]. Journal of Hazardous Materials,2011,190(1-3):897-902.
[40] Zhou W J,Chen C P,Lou L J,et al. Formation potential of nine nitrosamines from corresponding secondary amines by chloramination[J]. Chemosphere,2014,95:81-87.
[41]陈贻龙.地下式MBR工艺在广州京溪污水处理厂的应用[J].给水排水,2010,36(7):51-54.Chen Y L. Application of underground MBR in Guangzhou Jingxi wastewater treatment plant[J]. Water&Wastewater Engineering,2010,36(7):51-54.
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