洞庭湖不同营养级鱼组织中PCBs的分布特征
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摘要
采用稳定同位素分析技术和气相色谱-高分辨质谱联用技术,测定了洞庭湖6种鱼组织的稳定氮同位素丰度值(δ~(15)N值)和多氯联苯(PCBs)的含量,研究了鱼组织中PCBs分布特征及其与营养级的相关性.结果表明,∑PCBs115的浓度范围为0.04～9.77ng/g湿重,在鲤鱼性腺组织中最高.毒性当量为:0.0003～2.39pg/g湿重,在鳡鱼脂肪组织中最高.洞庭湖鱼中PCBs的含量处于较低水平.PCB28,52,95,99,101,105,110,118,138,153,155和209在所有组织中检出.Co-PCBs,Ind-PCBs和PCB209具有组织分布特异性.不同计量方式下,鱼组织中PCBs与δ~(15)N值具有相关性的同类物不同.
The toxicity of polychlorinated biphenyls(PCBs) and their transformation have been intensively investigated in recent years. However, the potential mechanisms of biotransformation in a lake food web remain unclear. In current study, the distribution characteristics of PCBs and δ~(15)N values in different tissues of six species of fishes, collected in Dongting Lake, were analysed with gas chromatography-high resolution mass spectrometer and stable isotope mass spectrometer, respectively. The correlation between PCBs and the trophic level were explored based on the concentrations and δ~(15)N values. The concentration of ∑PCBs115 ranged from 0.04 to 9.77 ng/g wet weight(ww), and the highest level was found in the gonad of Cyprinus carpio. The concentration of toxicity equivalent(TEQ) varied from 0.003 to 2.39 pg/g, with highest level detected in the fat of Silurus asotus. And the PCB levels in fish collected from Dongting Lake were at low level comparing with previous study. PCB28, 52, 95, 99, 101, 105, 110, 118, 138, 153, 155 and 209 were found in all tissues. The coplanar PCBs(Co-PCBs), Ind-PCBs(Indicator PCBs) and PCB209 was in a tissue-specific manner. The significant positive correlation(P<0.05) between the PCB congeners and δ~(15)N values varied depending on the calculation mode of PCB concentrations(such as, ng/g ww, ng/g dry weight and lipidnormalized).
The toxicity of polychlorinated biphenyls(PCBs) and their transformation have been intensively investigated in recent years. However, the potential mechanisms of biotransformation in a lake food web remain unclear. In current study, the distribution characteristics of PCBs and δ~(15)N values in different tissues of six species of fishes, collected in Dongting Lake, were analysed with gas chromatography-high resolution mass spectrometer and stable isotope mass spectrometer, respectively. The correlation between PCBs and the trophic level were explored based on the concentrations and δ~(15)N values. The concentration of ∑PCBs115 ranged from 0.04 to 9.77 ng/g wet weight(ww), and the highest level was found in the gonad of Cyprinus carpio. The concentration of toxicity equivalent(TEQ) varied from 0.003 to 2.39 pg/g, with highest level detected in the fat of Silurus asotus. And the PCB levels in fish collected from Dongting Lake were at low level comparing with previous study. PCB28, 52, 95, 99, 101, 105, 110, 118, 138, 153, 155 and 209 were found in all tissues. The coplanar PCBs(Co-PCBs), Ind-PCBs(Indicator PCBs) and PCB209 was in a tissue-specific manner. The significant positive correlation(P<0.05) between the PCB congeners and δ~(15)N values varied depending on the calculation mode of PCB concentrations(such as, ng/g ww, ng/g dry weight and lipidnormalized).
引文
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[15]Wolschke H,Meng X Z,Xie Z,et al.Novel flame retardants(N-FRs),polybrominated diphenyl ethers(PBDEs)and dioxin-like polychlorinated biphenyls(DL-PCBs)in fish,penguin,and skua from King George Island,Antarctica[J].Marine Pollution Bulletin,2015,96(1/2):513-518.
[16]王莎莎,高丽荣,田益玲,等.渤海湾海域10种鱼类中二噁英类及指示性多氯联苯的污染特征研究及风险评价[J].环境科学,2014,35(6):2281-2286.Wang S S,Gao L R,Tian Y L,et al.Levels distribution and risk assessment of the indicator and dioxin-like polychlorinated biphenyls in ten different species of marine fish of Bohai Bay,China[J].Environmental Science,2014,35(6):2281-2286.
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[19]Szlinder-Richert J,Barska I,Usydus Z,et al.Investigation of PCDD/Fs and dl-PCBs in fish from the southern Baltic Sea during the2002-2006period[J].Chemosphere,2009,74(11):1509-1515.
[20]Bordajandi L R,Martín I,Abad E,et al.Organochlorine compounds(PCBs,PCDDs and PCDFs)in seafish and seafood from the Spanish Atlantic Southwest Coast[J].Chemosphere,2006,64(9):1450-1457.
[21]Bocio A,Domingo J L,FalcóG,et al.Concentrations of PCDD/PCDFs and PCBs in fish and seafood from the Catalan(Spain)market:Estimated human intake[J].Environment International,2007,33(2):170-175.
[22]Costopoulou D,Vassiliadou I,Leondiadis L.PCDDs,PCDFs and PCBs in farmed fish produced in Greece:Levels and human population exposure assessment[J].Chemosphere,2016,146:511-518.
[23]耿婧婧.中国沿海地区鱼体中持久性有机氯污染物的分布特征及健康风险评估[D].上海:华东师范大学,2015.Geng J J.Distribution and human health risk assessment of persistent organochlorine contaminants in fish from Chinese coastal areas[D].Shanghai:East China Normal University,2015.
[24]胡国成,李雪梅,彭晓武,等.白洋淀鱼类体内多氯联苯积累特征及其毒性评价[J].农业环境科学学报,2012,31(4):667-672.Hu G C,Li X M,Peng X W,et al.Bioaccumulation and toxicity assessment of polychlorinated biphenyls in freshwater fish from Baiyangdian Lake,North China[J].Journal of Agro-Environment Science,2012,31(4):667-672.
[25]李娜.多氯联苯在水生食物链中的生物毒性及富集效应研究[D].广州:暨南大学,2012.Li N.Toxicity effects and enrichment effects of PCBs in the aquatic food chain[D].Guangzhou:Jinnan University,2012.
[26]Guruge K S,Tanabe S.Congener specific accumulation and toxic assessment of polychlorinated biphenyls in common cormorants,Phalacrocorax carbo,from Lake Biwa,Japan[J].Environmental Pollution,1997,96(3):425.
[27]叶玫,吴成业,余颖,等.福建省养殖大黄鱼中指示性多氯联苯残留水平及人体暴露风险评估[J].海洋科学,2011,35(11):63-68.Y M,Wu C Y,Yu Y,et al.Residues of Indicator-PCBs and risk assessment of human exposure in cultured large yellow croakers in Fujian Province[J].Marine sciences,2011,35(11):63-68.
[28]林光辉.稳定同位素生态学[M].北京:高等教育出版社,2013:162.Lin G H.Stable isotope ecology[M].Beijing:Higher Education Press,2013:162.
[29]Svensson E,Freitas V,Schouten S,et al.Comparison of the stable carbon and nitrogen isotopic values of gill and white muscle tissue of fish[J].Journal of Experimental Marine Biology&Ecology,2014,457(8):173-179.
[30]肖协文,王玉玉,张欢,等.饶河枯水期主要鱼类营养级位置及其影响因素[J].生态学报,2015,35(18):6216-6223.Xiao X W,Wang Y Y,Zhang H,et al.Trophic position and its impact on fish in Raohe River during the dry season,Jiangxi Province[J].Acta Ecologica Sinica,2015,35(18):6216-6223.
[2]胡晴晖.湄洲湾水体中持久性有机污染物的污染特征与风险评估[J].中国环境科学,2014,34(10):2536-2544.Hu Q H.Occurrence and ecological risk assessment of persistent organic pollutants in Meizhou Bay[J].China Environmental Science,2014,34(10):2536-2544.
[3]铁晓威,沈海涛,韩见龙,等.浙江省部分地区淡水鱼中多氯联苯污染研究[J].中国卫生检验杂志,2005,15(10):1241-1242.Tie X W,Shen H T,Han J L,et.al.Studies on PCBs of freshwater fish in some areas of Zhejiang Province[J].Chinese Journal of Health Laboratory Technology,2005,15(10):1241-1242.
[4]白红妍,韩彬,徐亚岩,等.桑沟湾经济贝类有机氯农药和多氯联苯残留水平及分布特征[J].海洋科学,2013,37(7):47-52.Bai H Y,Han B,Xu Y Y,et al.Residues and distribution characteristics of organochlorine pesticides and PCBs in economic shellfish in Sanggou Bay[J].Marine science,2013,37(7):47-52.
[5]卢双,张旭,裴晋,等.黄河中下游流域表层土壤中多氯联苯的残留特征[J].中国环境科学,2016,36(9):2741-2748.Lu S,Zhang X,Pei J,et al.Residual characteristics of polychlorinated biphenyls in surface soil of the Middle and Lower Reaches of the Yellow River[J].China Environmental Science,2016,36(9):2741-2748.
[6]梅卫平,阮慧慧,吴昊,等.滴水湖水系表层沉积物中多氯联苯残留与风险评价[J].中国环境科学,2014,34(8):2086-2092.Mei W P,Ruan H H,Wu H,et al.Residual characteristics and ecological risk assessment of polychlorinated biphenyls(PCBs)in the surface sediments of Dishui Lake watershed[J].China Environmental Science,2014,34(8):2086-2092.
[7]Batang Z B,Alikunhi N,Gochfeld,M,et al.Congener-specific levels and patterns of polychlorinated biphenyls in edible fish tissue from the central Red Sea coast of Saudi Arabia[J].Science of the Total Environment,2016,572:915-925.
[8]Wu W L,Deng X L,Zhou S J,et al.Levels,congener profiles,and dietary intake assessment of polychlorinated dibenzo-p-dioxins/dibenzofurans and dioxin-like polychlorinated biphenyls in beef,freshwater fish,and pork marketed in Guangdong Province,China[J].Science of the Total Environment 2017,615:412-421.
[9]Bodin N,Tapie N,Ménach K L,et al.PCB contamination in fish community from the Gironde Estuary(France):Blast from the past[J].Chemosphere,2014,98:66-72.
[10]Dufour E,Gerdeaux D,Corvi C,et al.Assessment of the contaminant concentration variability among Lake Geneva Arctic char using stable isotopic composition(δ15N andδ13C)[J].Environmental Toxicology:An International Journal,2001,16(2):185-191.
[11]Takahashi S,Oshihoi T,Ramu K,et al.Organohalogen compounds in deep-sea fishes from the western North Pacific,off-Tohoku,Japan:contamination status and bioaccumulation profiles[J].Marine pollution bulletin,2010,60(2):187-196.
[12]Zhao X R,Cui T T,Guo R,et al.A clean-up method for determination of multi-classes of persistent organic pollutants in sediment and biota samples with an aliquot sample[J].Analytica chimica acta,2019,1047:71-80.
[13]杨永亮,潘静,朱晓华,等.青岛及崇明岛食用鱼和鸭中共平面多氯联苯与多氯萘的研究[J].环境科学研究,2009,22(2):187-193.Yang Y L,Pan J,Zhu X H,et al.Studies on Coplanar-PCBs and PCNs in Edible Fish and Duck in Qingdao and Chongming Island[J].Rsearch of Environmental Sciences,2009,22(2):187-193.
[14]张中华,金士威,杨炜萍.市售鲫鱼体内多氯联苯污染水平及健康风险评估[J].湖北农业科学,2011,50(11):2287-2291.Zhang Z H,Jin S W,Yang W P.Concentration and health risk appraisal of polychlorinated biphenyls in crucian carp from market[J].Hubei Agricultural Sciences,2011,50(11):2287-2291.
[15]Wolschke H,Meng X Z,Xie Z,et al.Novel flame retardants(N-FRs),polybrominated diphenyl ethers(PBDEs)and dioxin-like polychlorinated biphenyls(DL-PCBs)in fish,penguin,and skua from King George Island,Antarctica[J].Marine Pollution Bulletin,2015,96(1/2):513-518.
[16]王莎莎,高丽荣,田益玲,等.渤海湾海域10种鱼类中二噁英类及指示性多氯联苯的污染特征研究及风险评价[J].环境科学,2014,35(6):2281-2286.Wang S S,Gao L R,Tian Y L,et al.Levels distribution and risk assessment of the indicator and dioxin-like polychlorinated biphenyls in ten different species of marine fish of Bohai Bay,China[J].Environmental Science,2014,35(6):2281-2286.
[17]Naito W,Jin J,Kang Y S,et al.Dynamics of PCDDs/DFs and coplanar-PCBs in an aquatic food chain of Tokyo Bay[J].Chemosphere,2003,53(4):347-362.
[18]Cariou R,Marchand P,Vénisseau A,et al.Prediction of the PCDD/Fand dl-PCB 2005-WHO-TEQ content based on the contribution of six congeners:Toward a new screening approach for fish samples[J].Environmental Pollution,2010,158(3):941-947.
[19]Szlinder-Richert J,Barska I,Usydus Z,et al.Investigation of PCDD/Fs and dl-PCBs in fish from the southern Baltic Sea during the2002-2006period[J].Chemosphere,2009,74(11):1509-1515.
[20]Bordajandi L R,Martín I,Abad E,et al.Organochlorine compounds(PCBs,PCDDs and PCDFs)in seafish and seafood from the Spanish Atlantic Southwest Coast[J].Chemosphere,2006,64(9):1450-1457.
[21]Bocio A,Domingo J L,FalcóG,et al.Concentrations of PCDD/PCDFs and PCBs in fish and seafood from the Catalan(Spain)market:Estimated human intake[J].Environment International,2007,33(2):170-175.
[22]Costopoulou D,Vassiliadou I,Leondiadis L.PCDDs,PCDFs and PCBs in farmed fish produced in Greece:Levels and human population exposure assessment[J].Chemosphere,2016,146:511-518.
[23]耿婧婧.中国沿海地区鱼体中持久性有机氯污染物的分布特征及健康风险评估[D].上海:华东师范大学,2015.Geng J J.Distribution and human health risk assessment of persistent organochlorine contaminants in fish from Chinese coastal areas[D].Shanghai:East China Normal University,2015.
[24]胡国成,李雪梅,彭晓武,等.白洋淀鱼类体内多氯联苯积累特征及其毒性评价[J].农业环境科学学报,2012,31(4):667-672.Hu G C,Li X M,Peng X W,et al.Bioaccumulation and toxicity assessment of polychlorinated biphenyls in freshwater fish from Baiyangdian Lake,North China[J].Journal of Agro-Environment Science,2012,31(4):667-672.
[25]李娜.多氯联苯在水生食物链中的生物毒性及富集效应研究[D].广州:暨南大学,2012.Li N.Toxicity effects and enrichment effects of PCBs in the aquatic food chain[D].Guangzhou:Jinnan University,2012.
[26]Guruge K S,Tanabe S.Congener specific accumulation and toxic assessment of polychlorinated biphenyls in common cormorants,Phalacrocorax carbo,from Lake Biwa,Japan[J].Environmental Pollution,1997,96(3):425.
[27]叶玫,吴成业,余颖,等.福建省养殖大黄鱼中指示性多氯联苯残留水平及人体暴露风险评估[J].海洋科学,2011,35(11):63-68.Y M,Wu C Y,Yu Y,et al.Residues of Indicator-PCBs and risk assessment of human exposure in cultured large yellow croakers in Fujian Province[J].Marine sciences,2011,35(11):63-68.
[28]林光辉.稳定同位素生态学[M].北京:高等教育出版社,2013:162.Lin G H.Stable isotope ecology[M].Beijing:Higher Education Press,2013:162.
[29]Svensson E,Freitas V,Schouten S,et al.Comparison of the stable carbon and nitrogen isotopic values of gill and white muscle tissue of fish[J].Journal of Experimental Marine Biology&Ecology,2014,457(8):173-179.
[30]肖协文,王玉玉,张欢,等.饶河枯水期主要鱼类营养级位置及其影响因素[J].生态学报,2015,35(18):6216-6223.Xiao X W,Wang Y Y,Zhang H,et al.Trophic position and its impact on fish in Raohe River during the dry season,Jiangxi Province[J].Acta Ecologica Sinica,2015,35(18):6216-6223.