中山市河涌水体及污水处理厂中合成麝香的分布规律
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摘要
对中山市5个区域的48条主要河涌水体与2间污水处理厂各工艺流程水体进行样品采集,运用固相微萃取进行前处理并结合气相色谱—质谱联用技术,检测各样品中佳乐麝香、吐纳麝香和酮麝香这3种合成麝香的含量,并分析其分布特征以及探讨污水处理厂处理工艺中合成麝香的浓度变化规律。结果表明:1)合成麝香已经普遍存在于中山市的河涌水体中。中山市西部地区和南部地区的河涌水体中合成麝香总含量相对其他区域最低,中部地区河涌水体中合成麝香含量亦较低。2)中山市雁企涌和魁魁涌等28条河涌水体中的主要合成麝香为佳乐麝香,一埒涌和乌沙涌等13条河涌水体的主要合成麝香为酮麝香,仅有苏埒涌和石军涌等7条河涌水体的主要合成麝香为佳乐麝香和酮麝香这2种合成麝香。3)氧化沟和A2/O工艺均能对合成麝香产生一定的去除效果。污水处理厂A对佳乐麝香、吐纳麝香和酮麝香的去除率分别为86.94%、72.15%和89.36%;而污水处理厂B对以上3种合成麝香的去除率分别为82.09%、85.73%和87.90%。4)2间污水处理厂的二沉池以及污水处理厂A的紫外消毒亦可对合成麝香产生进一步的去除效果;2间污水处理厂均能对酮麝香产生比佳乐麝香和吐纳麝香更高的去除率。
Water samples were collected from 48 main sewage streams and each process of 2 wastewater treatment plants in 5 regions of Zhongshan City. This study used Solid Phase MicroExtraction(SPME) for pretreatment and combined with Gas Chromatography/Mass Spectrometry(GC/MS) technique to detect the contents of three synthetic musks in the water samples. The three synthetic musks are Galaxolide(HHCB), Tonalide(AHTN) and Musk Ketone(MK). And the distribution characteristics of them were analyzed, as well as the change law of their concentrations along the water treatment processes of wastewater treatment plants, which had certain reference value for understanding the distribution of synthetic musks in sewage streams. The results showed: 1) Synthetic musks had been widely found in the sewage streams of Zhongshan City. Among them, the total contents of synthetic musks in 4 sewage streams, such as Yanqi Stream and Kuikui Stream, all exceeded 500 ng/L. The total contents of synthetic musks in 8 sewage streams, such as Huangpu Stream and Hengli Stream, were in the range of 200 – 500 ng/L. The total contents of synthetic musks in the remaining 36 sewage streams, such as Sulie Stream and Shijun Stream, were less than 200 ng/L. The total contents of synthetic musks from sewage streams in the Western and Southern regions of Zhongshan City were relatively the lowest as compared with other regions, due to their proximity to the outer river channels which could dilute and migrate pollutants, including synthetic musks. The Central Region also had low concentrations of synthetic musks in the sewage streams, which could be explained by that there were many wastewater treatment plants and the sewage collection rate was higher than that in other regions. 2) The major synthetic musk of different sewage streams was different. The main synthetic musk was HHCB, which accounted for more than 50% of total synthetic musks content in 28 sewage streams, such as Yanqi Stream and Kuikui Stream. The main synthetic musk was MK, which also accounted for more than 50% of total synthetic musks content in 13 sewage streams, such as Yilie Stream and Wusha Stream. And the main synthetic musks were HHCB and MK, which accounted for more than 35% of total synthetic musks content respectively in the other 7 sewage streams, such as Sulie Stream and Shijun Stream. 3) The Oxidation Ditch Process and Anaerobic/Anoxic/Oxic(A2/O) Process both could produce a certain removal effect on synthetic musks, due to activated sludge adsorption and microbial metabolic decomposition. In Wastewater Treatment Plant A, the ultimate removal rates of HHCB, AHTN and MK were 86.94%, 72.15% and 89.36%, respectively. In Wastewater Treatment Plant B, the ultimate removal rates of HHCB, AHTN and MK were 82.09%, 85.73% and 87.90%, respectively. 4) The secondary sedimentation tank of these two wastewater treatment plants and ultraviolet disinfection of Wastewater Treatment Plant A could produce further removal effects on synthetic musks. Both Wastewater Treatment Plant A and B could produce a higher removal rate on MK than HHCB and AHTN, which could be due to that MK contained nitrogen element and had a better removal effect.
Water samples were collected from 48 main sewage streams and each process of 2 wastewater treatment plants in 5 regions of Zhongshan City. This study used Solid Phase MicroExtraction(SPME) for pretreatment and combined with Gas Chromatography/Mass Spectrometry(GC/MS) technique to detect the contents of three synthetic musks in the water samples. The three synthetic musks are Galaxolide(HHCB), Tonalide(AHTN) and Musk Ketone(MK). And the distribution characteristics of them were analyzed, as well as the change law of their concentrations along the water treatment processes of wastewater treatment plants, which had certain reference value for understanding the distribution of synthetic musks in sewage streams. The results showed: 1) Synthetic musks had been widely found in the sewage streams of Zhongshan City. Among them, the total contents of synthetic musks in 4 sewage streams, such as Yanqi Stream and Kuikui Stream, all exceeded 500 ng/L. The total contents of synthetic musks in 8 sewage streams, such as Huangpu Stream and Hengli Stream, were in the range of 200 – 500 ng/L. The total contents of synthetic musks in the remaining 36 sewage streams, such as Sulie Stream and Shijun Stream, were less than 200 ng/L. The total contents of synthetic musks from sewage streams in the Western and Southern regions of Zhongshan City were relatively the lowest as compared with other regions, due to their proximity to the outer river channels which could dilute and migrate pollutants, including synthetic musks. The Central Region also had low concentrations of synthetic musks in the sewage streams, which could be explained by that there were many wastewater treatment plants and the sewage collection rate was higher than that in other regions. 2) The major synthetic musk of different sewage streams was different. The main synthetic musk was HHCB, which accounted for more than 50% of total synthetic musks content in 28 sewage streams, such as Yanqi Stream and Kuikui Stream. The main synthetic musk was MK, which also accounted for more than 50% of total synthetic musks content in 13 sewage streams, such as Yilie Stream and Wusha Stream. And the main synthetic musks were HHCB and MK, which accounted for more than 35% of total synthetic musks content respectively in the other 7 sewage streams, such as Sulie Stream and Shijun Stream. 3) The Oxidation Ditch Process and Anaerobic/Anoxic/Oxic(A2/O) Process both could produce a certain removal effect on synthetic musks, due to activated sludge adsorption and microbial metabolic decomposition. In Wastewater Treatment Plant A, the ultimate removal rates of HHCB, AHTN and MK were 86.94%, 72.15% and 89.36%, respectively. In Wastewater Treatment Plant B, the ultimate removal rates of HHCB, AHTN and MK were 82.09%, 85.73% and 87.90%, respectively. 4) The secondary sedimentation tank of these two wastewater treatment plants and ultraviolet disinfection of Wastewater Treatment Plant A could produce further removal effects on synthetic musks. Both Wastewater Treatment Plant A and B could produce a higher removal rate on MK than HHCB and AHTN, which could be due to that MK contained nitrogen element and had a better removal effect.
引文
Arthur C L and Pawliszyn J.1990.Solid phase microextraction with thermal desorption using fused silica optical fibers.Analytical Chemistry,62(19):2145-2148.
陈春,周启星,刘潇威,李松.2012.多环麝香对蚯蚓的急性和亚急性毒性效应.生态毒理学报,7(4):401-407.[Chen Chun,Zhuo Qixing,Liu Xiaowei and Li Song.2012.Acute and sub-acute toxicological effects of Polycyclic Musks on Earth-worm,Eisenia fetida.Asian Journal of Ecotoxicology,7(4):401-407.]
陈多宏,胡学玲,盛彦清,曾祥英,毕新慧,盛国英,傅家谟.2009.典型污水处理厂中多环麝香的污染特征.生态环境学报,18(1):101-105.[Chen Duohong,Hu Xueling,Sheng Yanqing,Zeng Xiangying,Bi Xinhui,Sheng Guoying and Fu Jiamo.2009.The Occurrence of Polycyclic Musks in a Typically Wastewater Treatment Plant.Ecology and Environmental Sciences,18(1):101-105.]
Carlsson G,?rn S,Andersson P L,S?derstr?m H and Norrgren L.2000.The impact of musk ketone on reproduction in zebrafish(Danio rerio).Marine Environmental Research,50(1/5):237-241.
Horii Y,Reiner J L,Loganathan B G,Kumar K S,Sajwan K and Kannan K.2007.Occurrence and fate of polycyclic musks in wastewater treatment plants in Kentucky and Georgia,USA.Chemosphere,68(11):2011-2020.
金鑫.2014.我国城市污水处理工艺及基本原理浅析.科技与企业,(5):147.[Jin Xin.2014.Analysis of Urban Sewage Treatment Technology and Basic Principles in China.Science Technology&Enterprises,(5):147.]
刘劲松.2012.典型河网区城市地表水污染特征研究--以广州为例.北京:中国科学院大学.[Liu Jinsong.2012.Water pollution characteristics of urban surface water in typical river network area-ACase Study of Guangzhou.Beijing:University of Chinese Academy of Sciences.]
李卓娜,周群芳,刘稷燕,史亚利,蔡亚岐,江桂斌.2012.多环麝香(PCMs)的环境行为及毒性效应.化学进展,24(4):606-615.[Li Zhuona,Zhou Qunfang,Liu Jiyan,Shi Yali,Cai Yaqi and Jiang Guibin.2012.Environmental Behavior and Toxicological Effects of Polycyclic Musks.Progress in Chemistry,24(4):606-615.]
Mersch-Sundermann V,Schneider H,Freywald C,Jenter C,Parzefall W and Knasmüller S.2001.Musk ketone enhances benzo(a)pyrene induced mutagenicity in human derived Hep G2 cells.Mutation Research,495(1):89-96.
Peck A M and Hornbuckle K C.2004.Synthetic Musk Fragrances in Lake Michigan.Environmental Science&Technology,38(2):367-372.
Reiner J L and Kannan K.2006.A survey of polycyclic musks in selected household commodities from the United States.Chemosphere,62(6):867-873.
Rimkus G G.1999.Polycyclic musk fragrances in the aquatic environment.Toxicology Letters,111(1):37-56.
Sanchez-Prado L,Lourido M,Lores M,Llompart,M,Garcia-Jares C and Cela R.2004.Study of the photoinduced degradation of polycyclic musk compounds by solid-phase microextraction and gas chromatography/mass spectrometry.Rapid Commun Mass Spectrom,18(11):1186-1192.
Skladanowski A C,Stepnowski P,Kleszczyński K and Dmochowska B.2005.AMP deaminase in vitro inhibition by xenobiotics A potential molecular method for risk assessment of synthetic nitro-and polycyclic musks,imidazolium ionic liquids and N-glucopyranosyl ammonium salts.Environmental toxicology and pharmacology,19(2):291-296.
Staci L S,William M B,Greet D A and William S E.2014.Trace analysis of fragrance materials in wastewater and treated wastewater.Environmental Science&Technology,34(6):959-965.
Stevens J L,Northcott G L,Stern G A,Tomy G T and Jones K C.2003.PAHs,PCBs,PCNs,organochlorine pesticides,synthetic musks,and polychlorinated n-alkanes in U.K.sewage sludge:survey results and implications.Environmental Science&Technology,37(3):462-467.
田艺心,王美娥,陈卫平,汪自强.2011.污水和污泥中的人工合成麝香分析方法.生态学杂志,30(2):395-400.[Tian Yixin,Wang Meie,Chen Weiping and Wang Ziqiang.2011.Analytical Methods for Synthetic Musk in Wastewater and Sewage Sludge.Chinese Journal of Ecology,30(2):395-400.]
王冠.2016.麝香类香料的合成研究进展.香料香精化妆品,33(1):62-68,72.[Wang Guan.2016.The Progress on Synthetic Study of Musks.Flavour Fragrance Cosmetics,33(1):62-68,72.]
王冠男,汤桦,陈大舟,冯洁,李蕾.2012.顶空固相微萃取-气相色谱-质谱联用测定香水中5种合成麝香.色谱,30(2):135-140.[Wang Guannan,Tang Hua,Chen Dazhou,Feng Jie and Li Lei.2012.Determination of Five Synthetic Musks in Perfume by Headspace Solid-phase Microextraction and Gas Chromatographymass Spectrometry.Chinese Journal of Chromatography,30(2):135-140.]
王征.2013.气相色谱-负化学源质谱法测定化妆品中的硝基麝香类化合物.香料香精化妆品,30(1):28-32.[Wang Zheng.2013.Determination of Nitro-Musks in Cosmetics by Gas Chromatography/Negative Chemical Ionization Mass Spectrometry.Flavour Fragrance Cosmetics,30(1):28-32.]
夏丽华,王芳,薛云.2003.珠江三角洲中小城镇地表水污染分析研究--以中山市坦洲镇为例.热带地理,23(2):162-166.[Xia Lihua,Wang Fang and Xue Yun.2003.A Study on Surface Water Pollution in the Small-Middle Towns of the Pearl River Delta-A Case Study of Tanzhou Town of Zhongshan.Tropical Geography,23(2):162-166.]
谢柏希,曾思春.2015.某城镇污水厂A2/O工艺氨氮去除率高而总氮去除率低的探讨.资源节约与环保,(5):34-35.[Xie Baixi and Zeng Sichun.2015.Discussion on high ammonia nitrogen removal rate and low total nitrogen removal rate in A2/O process of a town sewage treatment plant.Resources Economization&Environmental Protection,(5):34-35.]
杨国华,周永章,陈庆秋.2006.珠江三角洲水资源可持续利用与管理研究述评.热带地理,26(1):18-22.[Yang Guohua,Zhou Yongzhang and Chen Qingqiu.2006.A Review of Studies on Sustainable Use and Management of Water Resources in the Pearl River Delta.Tropical Geography,26(1):18-22.]
阎俊秀,李琼,崔俭杰,赵玥.2011.二甲苯麝香和酮麝香的分析方法进展.上海应用技术学院学报(自然科学版),11(2):103-107.[Yan Junxiu,Li Qiong,Cui Jianjie and Zhao Yue.2011.Detection progress of Musk Xylene and Musk Ketone.Journal of Shanghai Institute of Technology(Natural Science),11(2):103-107.]
Zeng X,Sheng G,Xiong Y and Fu J.2005.Determination of polycyclic musks in sewage sludge from Guangdong,China using GC-EI-MS.Chemosphere,60(6):817-823.
Zhang X,Yao Y,Zeng X,Qian G and Guo Y.2008.Synthetic musks in the aquatic environment and personal care products in Shanghai,China.Chemosphere,72(10):1553-1558.
钟国平,曹小曙.2016.多中心城市中山市职住空间关系特征.热带地理,36(4):591-599.[Zhong Guoping and Cao Xiaoshu.2016.Spatial Pattern of Job-housing Relationship of Polycentric Cities:A Case of Zhongshan City.Tropical Geography,36(4):591-599.]
Zhou H,Huang X,Gao M and Wen X.2009.Distribution and elimination of polycyclic musks in three sewage treatment plants of Beijing,China.Journal of Environmental Sciences,21(5):561-567.
赵婷婷,范培成,姚立荣,闫刚,李定龙,张文艺.2011.氨化细菌对植物浮岛人工湿地中有机氮强化分解.农业工程学报,27(S1):223-226.[Zhao Tingting,Fan Peicheng,Yao Lirong,Yan Gang,LIDinglong and ZHANG Wenyi.2011.Ammonifying bacteria in plant floating island of constructed wetland for strengthening decomposition of organic nitrogen.Transactions of the CSAE,27(S1):223-226.]
赵伟.2016.多孔Ti基体PbO2阳极的制备及降解水体中麝香污染物的研究.上海:东华大学.[Zhao Wei.2016.Study on preparation and characterization of PbO2 anode based on porous titanium and its application in electro-catalytic degradation of musk pollution in aqueous solution.Shanghai:Donghua University.]
陈春,周启星,刘潇威,李松.2012.多环麝香对蚯蚓的急性和亚急性毒性效应.生态毒理学报,7(4):401-407.[Chen Chun,Zhuo Qixing,Liu Xiaowei and Li Song.2012.Acute and sub-acute toxicological effects of Polycyclic Musks on Earth-worm,Eisenia fetida.Asian Journal of Ecotoxicology,7(4):401-407.]
陈多宏,胡学玲,盛彦清,曾祥英,毕新慧,盛国英,傅家谟.2009.典型污水处理厂中多环麝香的污染特征.生态环境学报,18(1):101-105.[Chen Duohong,Hu Xueling,Sheng Yanqing,Zeng Xiangying,Bi Xinhui,Sheng Guoying and Fu Jiamo.2009.The Occurrence of Polycyclic Musks in a Typically Wastewater Treatment Plant.Ecology and Environmental Sciences,18(1):101-105.]
Carlsson G,?rn S,Andersson P L,S?derstr?m H and Norrgren L.2000.The impact of musk ketone on reproduction in zebrafish(Danio rerio).Marine Environmental Research,50(1/5):237-241.
Horii Y,Reiner J L,Loganathan B G,Kumar K S,Sajwan K and Kannan K.2007.Occurrence and fate of polycyclic musks in wastewater treatment plants in Kentucky and Georgia,USA.Chemosphere,68(11):2011-2020.
金鑫.2014.我国城市污水处理工艺及基本原理浅析.科技与企业,(5):147.[Jin Xin.2014.Analysis of Urban Sewage Treatment Technology and Basic Principles in China.Science Technology&Enterprises,(5):147.]
刘劲松.2012.典型河网区城市地表水污染特征研究--以广州为例.北京:中国科学院大学.[Liu Jinsong.2012.Water pollution characteristics of urban surface water in typical river network area-ACase Study of Guangzhou.Beijing:University of Chinese Academy of Sciences.]
李卓娜,周群芳,刘稷燕,史亚利,蔡亚岐,江桂斌.2012.多环麝香(PCMs)的环境行为及毒性效应.化学进展,24(4):606-615.[Li Zhuona,Zhou Qunfang,Liu Jiyan,Shi Yali,Cai Yaqi and Jiang Guibin.2012.Environmental Behavior and Toxicological Effects of Polycyclic Musks.Progress in Chemistry,24(4):606-615.]
Mersch-Sundermann V,Schneider H,Freywald C,Jenter C,Parzefall W and Knasmüller S.2001.Musk ketone enhances benzo(a)pyrene induced mutagenicity in human derived Hep G2 cells.Mutation Research,495(1):89-96.
Peck A M and Hornbuckle K C.2004.Synthetic Musk Fragrances in Lake Michigan.Environmental Science&Technology,38(2):367-372.
Reiner J L and Kannan K.2006.A survey of polycyclic musks in selected household commodities from the United States.Chemosphere,62(6):867-873.
Rimkus G G.1999.Polycyclic musk fragrances in the aquatic environment.Toxicology Letters,111(1):37-56.
Sanchez-Prado L,Lourido M,Lores M,Llompart,M,Garcia-Jares C and Cela R.2004.Study of the photoinduced degradation of polycyclic musk compounds by solid-phase microextraction and gas chromatography/mass spectrometry.Rapid Commun Mass Spectrom,18(11):1186-1192.
Skladanowski A C,Stepnowski P,Kleszczyński K and Dmochowska B.2005.AMP deaminase in vitro inhibition by xenobiotics A potential molecular method for risk assessment of synthetic nitro-and polycyclic musks,imidazolium ionic liquids and N-glucopyranosyl ammonium salts.Environmental toxicology and pharmacology,19(2):291-296.
Staci L S,William M B,Greet D A and William S E.2014.Trace analysis of fragrance materials in wastewater and treated wastewater.Environmental Science&Technology,34(6):959-965.
Stevens J L,Northcott G L,Stern G A,Tomy G T and Jones K C.2003.PAHs,PCBs,PCNs,organochlorine pesticides,synthetic musks,and polychlorinated n-alkanes in U.K.sewage sludge:survey results and implications.Environmental Science&Technology,37(3):462-467.
田艺心,王美娥,陈卫平,汪自强.2011.污水和污泥中的人工合成麝香分析方法.生态学杂志,30(2):395-400.[Tian Yixin,Wang Meie,Chen Weiping and Wang Ziqiang.2011.Analytical Methods for Synthetic Musk in Wastewater and Sewage Sludge.Chinese Journal of Ecology,30(2):395-400.]
王冠.2016.麝香类香料的合成研究进展.香料香精化妆品,33(1):62-68,72.[Wang Guan.2016.The Progress on Synthetic Study of Musks.Flavour Fragrance Cosmetics,33(1):62-68,72.]
王冠男,汤桦,陈大舟,冯洁,李蕾.2012.顶空固相微萃取-气相色谱-质谱联用测定香水中5种合成麝香.色谱,30(2):135-140.[Wang Guannan,Tang Hua,Chen Dazhou,Feng Jie and Li Lei.2012.Determination of Five Synthetic Musks in Perfume by Headspace Solid-phase Microextraction and Gas Chromatographymass Spectrometry.Chinese Journal of Chromatography,30(2):135-140.]
王征.2013.气相色谱-负化学源质谱法测定化妆品中的硝基麝香类化合物.香料香精化妆品,30(1):28-32.[Wang Zheng.2013.Determination of Nitro-Musks in Cosmetics by Gas Chromatography/Negative Chemical Ionization Mass Spectrometry.Flavour Fragrance Cosmetics,30(1):28-32.]
夏丽华,王芳,薛云.2003.珠江三角洲中小城镇地表水污染分析研究--以中山市坦洲镇为例.热带地理,23(2):162-166.[Xia Lihua,Wang Fang and Xue Yun.2003.A Study on Surface Water Pollution in the Small-Middle Towns of the Pearl River Delta-A Case Study of Tanzhou Town of Zhongshan.Tropical Geography,23(2):162-166.]
谢柏希,曾思春.2015.某城镇污水厂A2/O工艺氨氮去除率高而总氮去除率低的探讨.资源节约与环保,(5):34-35.[Xie Baixi and Zeng Sichun.2015.Discussion on high ammonia nitrogen removal rate and low total nitrogen removal rate in A2/O process of a town sewage treatment plant.Resources Economization&Environmental Protection,(5):34-35.]
杨国华,周永章,陈庆秋.2006.珠江三角洲水资源可持续利用与管理研究述评.热带地理,26(1):18-22.[Yang Guohua,Zhou Yongzhang and Chen Qingqiu.2006.A Review of Studies on Sustainable Use and Management of Water Resources in the Pearl River Delta.Tropical Geography,26(1):18-22.]
阎俊秀,李琼,崔俭杰,赵玥.2011.二甲苯麝香和酮麝香的分析方法进展.上海应用技术学院学报(自然科学版),11(2):103-107.[Yan Junxiu,Li Qiong,Cui Jianjie and Zhao Yue.2011.Detection progress of Musk Xylene and Musk Ketone.Journal of Shanghai Institute of Technology(Natural Science),11(2):103-107.]
Zeng X,Sheng G,Xiong Y and Fu J.2005.Determination of polycyclic musks in sewage sludge from Guangdong,China using GC-EI-MS.Chemosphere,60(6):817-823.
Zhang X,Yao Y,Zeng X,Qian G and Guo Y.2008.Synthetic musks in the aquatic environment and personal care products in Shanghai,China.Chemosphere,72(10):1553-1558.
钟国平,曹小曙.2016.多中心城市中山市职住空间关系特征.热带地理,36(4):591-599.[Zhong Guoping and Cao Xiaoshu.2016.Spatial Pattern of Job-housing Relationship of Polycentric Cities:A Case of Zhongshan City.Tropical Geography,36(4):591-599.]
Zhou H,Huang X,Gao M and Wen X.2009.Distribution and elimination of polycyclic musks in three sewage treatment plants of Beijing,China.Journal of Environmental Sciences,21(5):561-567.
赵婷婷,范培成,姚立荣,闫刚,李定龙,张文艺.2011.氨化细菌对植物浮岛人工湿地中有机氮强化分解.农业工程学报,27(S1):223-226.[Zhao Tingting,Fan Peicheng,Yao Lirong,Yan Gang,LIDinglong and ZHANG Wenyi.2011.Ammonifying bacteria in plant floating island of constructed wetland for strengthening decomposition of organic nitrogen.Transactions of the CSAE,27(S1):223-226.]
赵伟.2016.多孔Ti基体PbO2阳极的制备及降解水体中麝香污染物的研究.上海:东华大学.[Zhao Wei.2016.Study on preparation and characterization of PbO2 anode based on porous titanium and its application in electro-catalytic degradation of musk pollution in aqueous solution.Shanghai:Donghua University.]