黄河中游(渭南—郑州段)全/多氟烷基化合物的分布及通量
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摘要
本研究收集黄河中游(渭南—郑州段)表层水样品,利用高效液相色谱质谱串联的方法分析了水相和颗粒相中的28种全氟和多氟烷基化合物(PFASs).结果表明,水相和颗粒相中Σ28PFASs的含量分别为18.4~56.9 ng·L~(-1)和26.8~164ng·g~(-1)(以干重计).水相和颗粒相中以全氟己酸(PFHx A)为主要污染物,分别占总含量的27%和16%,且3H-全氟-3-(3-甲氧基丙氧基)丙酸(ADONA)、氯代多氟醚基磺酸(6∶2和8∶2 Cl-PFESA)在颗粒相均有检出,表明PFASs替代品的生产和使用逐渐增多.PFASs在水相-颗粒相中的lg Kd变化范围为2.95±0.553(PFPe A)~3.85±0.237(8∶2 FTUCA),颗粒物吸附氟调聚羧酸(FTCAs)和不饱和氟调聚羧酸(FTUCAs)的能力随碳链长度的增长而增加,全氟烷基磺酸(PFSAs)较全氟烷基羧酸(PFCAs)更容易被颗粒物吸附.黄河郑州—渭南段PFASs的通量呈现先降低后增加的趋势,表明该河段接纳了来自上游及支流的污染输入.此外,结果表明水相中的PFASs通量大于颗粒相.
Surface water samples were collected in the middle reaches of the Yellow River(Weinan-Zhengzhou section) and all 28 perfluoroalkyl and polyfluoroalkyl substance(PFAS) levels were measured using high-performance liquid chromatography-tandem mass spectrometry(HPLC-MS/MS).The results show that the levels of PFASs in the water and particle phase are 18.4-56.9 ng·L~(-1) and 26.8-164 ng·g~(-1),respectively.Perfluorohexanoic acid(PFHx A) in the water and particle phases is the main pollutant,accounting for 27% and 16% of the total concentrations,respectively,and 3 H-perfluoro-3-[(3-methoxy-propoxy)-propanoate] acid(ADONA)and chlorinated polyfluorinated ethersulfonic acids(6∶2 and 8∶2 Cl-PFESA) were detected in the particle phase,indicating that the use of PFAS alternatives gradually increases.The lg Kdof PFASs between the water and particle phase ranges from 2.95 ± 0.553(PFPe A) to 3.85 ± 0.237(8∶2 FTUCA) and the adsorption of fluorotelomer carboxylic acids(FTCAs) and fluorotelomer unsaturated carboxylic acids(FTUCAs) on particulate matter increases with increasing of carbon chain length.Perfluoroalkane sulfonic acids(PFSAs) are more easily adsorbed by particulate matter than perfluoroalkyl carboxylic acids(PFCAs).The fluxes of PFASs in the Weinan-Zhengzhou section of the Yellow River show a decrease at first and then increase,indicating that this section receives pollution inputs from the upstream and tributaries.In addition,the results show that the fluxes of PFASs in the water phase are greater than those in the particle phase.
Surface water samples were collected in the middle reaches of the Yellow River(Weinan-Zhengzhou section) and all 28 perfluoroalkyl and polyfluoroalkyl substance(PFAS) levels were measured using high-performance liquid chromatography-tandem mass spectrometry(HPLC-MS/MS).The results show that the levels of PFASs in the water and particle phase are 18.4-56.9 ng·L~(-1) and 26.8-164 ng·g~(-1),respectively.Perfluorohexanoic acid(PFHx A) in the water and particle phases is the main pollutant,accounting for 27% and 16% of the total concentrations,respectively,and 3 H-perfluoro-3-[(3-methoxy-propoxy)-propanoate] acid(ADONA)and chlorinated polyfluorinated ethersulfonic acids(6∶2 and 8∶2 Cl-PFESA) were detected in the particle phase,indicating that the use of PFAS alternatives gradually increases.The lg Kdof PFASs between the water and particle phase ranges from 2.95 ± 0.553(PFPe A) to 3.85 ± 0.237(8∶2 FTUCA) and the adsorption of fluorotelomer carboxylic acids(FTCAs) and fluorotelomer unsaturated carboxylic acids(FTUCAs) on particulate matter increases with increasing of carbon chain length.Perfluoroalkane sulfonic acids(PFSAs) are more easily adsorbed by particulate matter than perfluoroalkyl carboxylic acids(PFCAs).The fluxes of PFASs in the Weinan-Zhengzhou section of the Yellow River show a decrease at first and then increase,indicating that this section receives pollution inputs from the upstream and tributaries.In addition,the results show that the fluxes of PFASs in the water phase are greater than those in the particle phase.
引文
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[3]EPA.2010/15 PFOA stewardship program:guidance on reporting emissions and product content[R].EPA-HQ-OPPT-2006-0621,U.S.:Office of Pollution Prevention and Toxics,Environmental Protection Agency,2006.
[4]Zhao Z,Tang J H,Mi L J,et al.Perfluoroalkyl and polyfluoroalkyl substances in the lower atmosphere and surface waters of the Chinese Bohai Sea,Yellow Sea,and Yangtze River estuary[J].Science of the Total Environment,2017,599-600:114-123.
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[6]Conder J M,Hoke R A,de Wolf W,et al.Are PFCAs bioaccumulative?A critical review and comparison with regulatory criteria and persistent lipophilic compounds[J].Environmental Science&Technology,2008,42(4):995-1003.
[7]Kleszczyński K,Gardzielewski P,Mulkiewicz E,et al.Analysis of structure-cytotoxicity in vitro relationship(SAR)for perfluorinated carboxylic acids[J].Toxicology in Vitro,2007,21(6):1206-1211.
[8]Ruan T,Lin Y F,Wang T,et al.Identification of novel polyfluorinated ether sulfonates as PFOS alternatives in municipal sewage sludge in China[J].Environmental Science&Technology,2015,49(11):6519-6527.
[9]Higgins C P,Luthy R G.Sorption of perfluorinated surfactants on sediments[J].Environmental Science&Technology,2006,40(23):7251-7256.
[10]Chen H,Han J B,Zhang C,et al.Occurrence and seasonal variations of per-and polyfluoroalkyl substances(PFASs)including fluorinated alternatives in rivers,drain outlets and the receiving Bohai Sea of China[J].Environmental Pollution,2017,231(Pt 2):1223-1231.
[11]Chen H,Wang X M,Zhang C,et al.Occurrence and inputs of perfluoroalkyl substances(PFASs)from rivers and drain outlets to the Bohai Sea,China[J].Environmental Pollution,2017,221:234-243.
[12]Labadie P,Chevreuil M.Partitioning behaviour of perfluorinated alkyl contaminants between water,sediment and fish in the Orge River(nearby Paris,France)[J].Environmental Pollution,2011,159(2):391-397.
[13]Prevedouros K,Cousins I T,Buck R C,et al.Sources,fate and transport of perfluorocarboxylates[J].Environmental Science&Technology,2006,40(1):32-44.
[14]Zhao P J,Xia X H,Dong J W,et al.Short-and long-chain perfluoroalkyl substances in the water,suspended particulate matter,and surface sediment of a turbid river[J].Science of the Total Environment,2016,568:57-65.
[15]Zhang L L,Lee L S,Niu J F,et al.Kinetic analysis of aerobic biotransformation pathways of a perfluorooctane sulfonate(PFOS)precursor in distinctly different soils[J].Environmental Pollution,2017,229:159-167.
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[17]Ding G H,Peijnenburg W J G M.Physicochemical properties and aquatic toxicity of poly-and perfluorinated compounds[J].Critical Reviews in Environmental Science and Technology,2013,43(6):598-678.
[18]Viers J,DupréB,Gaillardet J.Chemical composition of suspended sediments in World Rivers:new insights from a new database[J].Science of the Total Environment,2009,407(2):853-868.
[19]刘昕宇,冯玉君,刘玲花,等.黄河重点河段水环境有毒有机物污染现状浅析[J].水资源保护,2004,20(2):37-38,56.Liu X Y,Feng Y J,Liu L H,et al.Current situation of toxic organism induced pollution in water environment of critical section of Yellow River[J].Water Resources Protection,2004,20(2):37-38,56.
[20]Ahrens L.Polyfluoroalkyl compounds in the aquatic environment:a review of their occurrence and fate[J].Journal of Environmental Monitoring,2011,13(1):20-31.
[21]Klaunig J E,Shinohara M,Iwai H,et al.Evaluation of the chronic toxicity and carcinogenicity of perfluorohexanoic acid(PFHx A)in Sprague-Dawley rats[J].Toxicologic Pathology,2015,43(2):209-220.
[22]Lu Z B,Song L N,Zhao Z,et al.Occurrence and trends in concentrations of perfluoroalkyl substances(PFASs)in surface waters of eastern China[J].Chemosphere,2015,119:820-827.
[23]Wang S W,Huang J,Yang Y,et al.First report of a Chinese PFOS alternative overlooked for 30 Years:its toxicity,persistence,and presence in the environment[J].Environmental Science&Technology,2013,47(18):10163-10170.
[24]Zhang L,Liu J G,Hu J X,et al.The inventory of sources,environmental releases and risk assessment for perfluorooctane sulfonate in China[J].Environmental Pollution,2012,165:193-198.
[25]Heydebreck F,Tang J H,Xie Z Y,et al.Alternative and legacy perfluoroalkyl substances:differences between european and Chinese River/Estuary systems[J].Environmental Science&Technology,2015,49(14):8386-8395.
[26]Fromme H,W9ckner M,Roscher E,et al.ADONA and perfluoroalkylated substances in plasma samples of German blood donors living in South Germany[J].International Journal of Hygiene and Environmental Health,2017,220(2 Pt B):455-460.
[27]Ding G H,Xue H H,Yao Z W,et al.Occurrence and distribution of perfluoroalkyl substances(PFASs)in the water dissolved phase and suspended particulate matter of the Dalian Bay,China[J].Chemosphere,2018,200:116-123.
[28]张智,曾晓岚,王利利,等.泥沙沉降对水库富营养化指标的影响[J].中国环境科学,2007,27(2):213-216.Zhang Z,Zeng X L,Wang L L,et al.The influence of sediment subsiding on the index of the reservoir eutrophication[J].China Environmental Science,2007,27(2):213-216.
[29]Ran X B,Yu Z G,Yao Q Z,et al.Silica retention in the Three Gorges Reservoir[J].Biogeochemistry,2013,112(1-3):209-228.
[30]Zhao X F,Zhang H J,Fan J F,et al.Dioxin-like compounds in sediments from the Daliao River Estuary of Bohai Sea:distribution and their influencing factors[J].Marine Pollution Bulletin,2011,62(5):918-925.
[31]Eriksson U,Krrman A.World-wide indoor exposure to polyfluoroalkyl phosphate esters(PAPs)and other PFASs in household dust[J].Environmental Science&Technology,2015,49(24):14503-14511.
[32]Zhao L J,Folsom P W,Wolstenholme B W,et al.6:2Fluorotelomer alcohol biotransformation in an aerobic river sediment system[J].Chemosphere,2013,90(2):203-209.
[33]Ellis D A,Martin J W,de Silva A O,et al.Degradation of fluorotelomer alcohols:a likely atmospheric source of perfluorinated carboxylic acids[J].Environmental Science&Technology,2004,38(12):3316-3321.
[34]Gebbink W A,Ullah S,Sandblom O,et al.Polyfluoroalkyl phosphate esters and perfluoroalkyl carboxylic acids in target food samples and packaging-method development and screening[J].Environmental Science and Pollution Research,2013,20(11):7949-7958.
[35]国家质量监督检验检疫总局.河南省食品相关产品行业生产及产品质量检测状况调研报告[EB/OL].http://www.aqsiq.gov.cn/xxgk_13386/zxxxgk/201401/t20140110_393632.htm,2014-01-10.
[36]Wang T Y,Khim J S,Chen C L,et al.Perfluorinated compounds in surface waters from Northern China:comparison to level of industrialization[J].Environment International,2012,42:37-46.
[37]Chen X W,Zhu L Y,Pan X Y,et al.Isomeric specific partitioning behaviors of perfluoroalkyl substances in water dissolved phase,suspended particulate matters and sediments in Liao River Basin and Taihu Lake,China[J].Water Research,2015,80:235-244.
[38]Li F S,Sun H W,Hao Z N,et al.Perfluorinated compounds in Haihe River and Dagu Drainage Canal in Tianjin,China[J].Chemosphere,2011,84(2):265-271.
[39]So M K,Miyake Y,Yeung W Y,et al.Perfluorinated compounds in the Pearl River and Yangtze River of China[J].Chemosphere,2007,68(11):2085-2095.
[40]Loos R,Gawlik B M,Locoro G,et al.EU-wide survey of polar organic persistent pollutants in European river waters[J].Environmental Pollution,2009,157(2):561-568.
[41]Wang S L,Wang H,Deng W J.Perfluorooctane sulfonate(PFOS)distribution and effect factors in the water and sediment of the Yellow River Estuary,China[J].Environmental Monitoring and Assessment,2013,185(10):8517-8524.
[42]陈欣维.全氟化合物支链/直链异构体在水体多界面分配行为的研究[D].天津:南开大学,2014.Chen X W.Distribution and partitioning behaviors of perfluoroalkyl substances and typical isomers in water[D].Tianjin:Nankai University,2014.
[43]Hu G Z,Wang H T,Fan X G,et al.Mathematical model of coalbed gas flow with Klinkenberg effects in multi-physical fields and its analytic solution[J].Transport in Porous Media,2009,76(3):407-420.
[44]Wang J Z,Guan Y F,Ni H G,et al.Polycyclic aromatic hydrocarbons in riverine runoff of the pearl river delta(China):concentrations,fluxes,and fate[J].Environmental Science&Technology,2007,41(16):5614-5619.
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