成都饮食中全氟化合物的污染特征及健康风险评估
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摘要
为了解成都市居民通过饮食暴露于全氟化合物(Perfluoroalkyl Substances, PFASs)的情况,本研究通过调查统计成都市居民的主要饮食情况,选取米、蔬菜、牛奶、鸡蛋、鱼和猪肉6类饮食为研究对象,采用超高效液相色谱-串联质谱法对样品中17种PFASs进行检测.结果显示,所有饮食中均检出PFASs,说明PFASs在饮食中普遍存在.鸡蛋中的∑PFASs含量最高,达(155±25.4) ng·g~(-1)(湿重,下同);白菜的∑PFASs含量最低,仅为(0.101±0.026) ng·g~(-1).大部分样品中以全氟辛烷羧酸(Perfluroroocantanoic Acid,PFOA)为主,其次为短碳链的全氟羧酸(Perfluoroalkyl Acids,PFCAs).其中,鸡蛋蛋黄中∑PFASs的含量为(600.0±98.6) ng·g~(-1),远高于蛋清中的含量(0.606±0.101) ng·g~(-1),且蛋黄中主要为全氟辛烷磺酸(Perfluorooctane Sulfonate,PFOS)(98.1%).通过风险评估可以得出,成都市居民对PFOS和PFOA的日摄入量分为85.6 ng·kg~(-1)·d~(-1)和4.38 ng·kg~(-1)·d~(-1),低于欧盟食品安全局推荐的每日最大摄入量,不会对成都市居民造成即时伤害.
Rice, vegetables, milk, eggs, fish and pork, which are the main dietarty for the general population living in Chengdu, were analyzed in the present study to reveal the risk of perfluoroalkyl substances(PFASs) exposure in Chengdu. Seventeen PFASs were analyzed by the ultra-performance liquid chromatography tandem mass spectrometry(UPLC-MS/MS). The results showed that all of the PFASs were detected in diet samples, suggesting widespread of PFASs in diets. In addition, eggs displayed the highest ∑PFAS levels, and reached to(155±25.4) ng·g~(-1)(wet weight, the same in the follows), while Chinese cabbage showed the lowest values(0.101±0.026) ng·g~(-1). Perfluroroocantanoic acid and short chained perfluoroalkyl acids were the predominant PFASs in most of the diet. Furthermore, ∑PFASs concentrations in egg yolk(600.0±98.6) ng·g~(-1) were extremely higher than that in eggs white(0.606±0.101) ng·g~(-1), and perfluorooctane sulfonate was the most important one in egg yolk(98.1%). Estimated daily intake via foods(EDI) showed that the EDI value of PFOS and PFOA were 85.6 ng·kg~(-1)·d~(-1) and 4.38 ng·kg~(-1)·d~(-1) respectively, lower than the tolerable daily intakes recommended by European Food Safety Authority, indicating that there was no instant health risk to local residents.
Rice, vegetables, milk, eggs, fish and pork, which are the main dietarty for the general population living in Chengdu, were analyzed in the present study to reveal the risk of perfluoroalkyl substances(PFASs) exposure in Chengdu. Seventeen PFASs were analyzed by the ultra-performance liquid chromatography tandem mass spectrometry(UPLC-MS/MS). The results showed that all of the PFASs were detected in diet samples, suggesting widespread of PFASs in diets. In addition, eggs displayed the highest ∑PFAS levels, and reached to(155±25.4) ng·g~(-1)(wet weight, the same in the follows), while Chinese cabbage showed the lowest values(0.101±0.026) ng·g~(-1). Perfluroroocantanoic acid and short chained perfluoroalkyl acids were the predominant PFASs in most of the diet. Furthermore, ∑PFASs concentrations in egg yolk(600.0±98.6) ng·g~(-1) were extremely higher than that in eggs white(0.606±0.101) ng·g~(-1), and perfluorooctane sulfonate was the most important one in egg yolk(98.1%). Estimated daily intake via foods(EDI) showed that the EDI value of PFOS and PFOA were 85.6 ng·kg~(-1)·d~(-1) and 4.38 ng·kg~(-1)·d~(-1) respectively, lower than the tolerable daily intakes recommended by European Food Safety Authority, indicating that there was no instant health risk to local residents.
引文
Chen X W,Zhu L Y,Pan X Y,et al.2015.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,80:235-244
Eriksson U,Karrman A,Rotander A,et al.2013.Perfluoroalkyl substances (PFASs) in food and water from Faroe Islands[J].Environ Sci Pollut Res Int,20(11):7940-7948
European Food Safety Authority (EFSA).2008.Perfluorooctane sulfonate (PFOS),perfluorooctanoic acid (PFOA) and their salts scientific opinion of the panel on contaminants in the food chain[J].EFSA Journal,6(7):653:1-131
Fang S H,Chen X W,Zhao S Y,et al.2014.Trophic magnification and isomer fractionation of perfluoroalkyl substances in the food web of Taihu Lake,China[J].Environmental Science & Technology,48(4):2173-2182
Fuentes S,Vicens P,Colomina M,et al.2007.Behavioral effects in adult mice exposed to perfluorooctane sulfonate (PFOS) [J].Toxicology,242(1/3):123-129
Gebbink W A,Letcher R J.2012.Comparative tissue and body compartment accumulation and maternal transfer to eggs of perfluoroalkyl sulfonates and carboxylates in Great Lakes herring gulls[J].Environmental Pollution,162:40-47
Gebbink W A,Van Asseldonk L,Van Leeuwen S P J.2017.Presence of emerging per- and polyfluoroalkyl substances (PFASs) in river and drinking water near a fluorochemical production plant in the Netherlands[J].Environmental Science & Technology,51(19):11057-11065
Giesy J P,Kannan K.2001.Global distribution of perfluorooctane sulfonate in wildlife[J].Environmental Science & Technology,35(7):1339-1342
Gulkowska A,Jiang Q T,So M K,et al.2006.Persistent perfluorinated acids in seafood collected from two cities of China [J].Environmental Science & Technology,40(12):3736-3741
Holmstrom K E,Berger U.2008.Tissue distribution of perfluorinated surfactants in common guillemot (Uria aalge) from the Baltic Sea[J].Environmental Science & Technology,42(16):5879-5884
Heydebreck F,Tang J,Xie Z,et al.2016.Emissions of per- and polyfluoroalkyl substances in a textile manufacturing plant in china and their relevance for workers′ exposure[J].Environmental Science & Technology,50(19):10386-10396
Jin H,Zhang Y,Zhu L,et al.2015.Isomer profiles of perfluoroalkyl substances in water and soil surrounding a Chinese Fluorochemical Manufacturing Park[J].Environmental Science & Technology,49(8):4946-4954
Kleszczynski K,Gardzielewski P,Mulkiewicz E,et al.2007.Analysis of structure-cytotoxicity in vitro relationship (SAR) for perfluorinated carboxylic acids [J].Toxicology in Vitro,21(6):1206-1211
Lau C,Anitole K,Hodes C,et al.2007.Perfluoroalkyl acids:A review of monitoring and toxicological findings[J].Toxicological Sciences,99(2):366-394
柳思帆,王铁宇,薛科社,等.2017.北京水源地鱼体全氟化合物的暴露水平及其健康风险[J].生态毒理学报,12(1):111-118
罗超.2014.福建省大米中全氟烷基化合物污染水平调查[D].厦门:集美大学
Lofstrand K,Jorundsdottir H,Tomy G,et al.2008.Spatial trends of polyfluorinated compounds in guillemot (Uria aalge) eggs from North-Western Europe[J].Chemosphere,72(10):1475-1480
Martin J W,Mabury S A,Solomon K R,et al.2003a.Bioconcentration and tissue distribution of perfluorinated acids in rainbow trout (Oncorhynchus mykiss)[J].Environmental Toxicology and Chemistry,22(1):196-204
Martin J W,Mabury S A,Solomon K R,et al.2003b.Dietary accumulation of perfluorinated acids in juvenile rainbow trout (Oncorhynchus mykiss)[J].Environmental Toxicology & Chemistry,22(1):189-195
Meesters R J W,Schr?der H F.2004.Perfluorooctane sulfonate - a quite mobile anionic anthropogenic surfactant,ubiquitously found in the environment[J].Water Science and Technology,50(5):235-242
Poothong S,Thomsen C,Padilla-Sanchez J A,et al.2017.Distribution of novel and well-known poly- and perfluoroalkyl substances (PFASs) in human serum,plasma,and whole blood[J].Environmental Science & Technology,51(22):13388-13396
Powley C R,George S W,Ryan T W,et al.2005.Matrix effect-free analytical methods for determination of perfluorinated carboxylic acids in environmental matrixes[J].Analytical Chemistry,77(19):6353-6358
Shan G,Wang Z,Zhou L,et al.2016.Impacts of daily intakes on the isomeric profiles of perfluoroalkyl substances (PFASs) in human serum[J].Environment International,89-90:62-70
Shi Y L,Pan Y Y,Wang J M,et al.2012.Distribution of perfluorinated compounds in water,sediment,biota and floating plants in Baiyangdian Lake,China[J].Journal of Environmental Monitoring,14(2):636-642
Taniyasu S,Kannan K,Horii Y,et al.2003.A survey of perfluorooctane sulfonate and related perfluorinated organic compounds in water,fish,birds,and humans from Japan[J].Environmental Science & Technology,37(12):2634-2639
US-EPA.2006.PFOA Stewardship Program[OL].2006-10-31.http://www.epa.gov/oppt/pfoa/pubs/stewardship/pfoastewardshipbasics.html
Wang J,Shi Y,Pan Y,et al.2010a.Perfluorinated compounds in milk,milk powder and yoghurt purchased from markets in China[J].Chinese Science Bulletin,55(11):1020-1025
Wang J,Shi Y,Pan Y,et al.2010b.Perfluorooctane sulfonate (PFOS) and other fluorochemicals in viscera and muscle of farmed pigs and chickens in Beijing,China[J].Chinese Science Bulletin,55(31):3550-3555
Wang Y,Yeung L,Yamashita N,et al.2008.Perfluorooctane sulfonate (PFOS) and related fluorochemicals in chicken egg in China[J].Chinese Science Bulletin,53(4):501-507
Winkens K,Koponen J,Schuster J,et al.2017.Perfluoroalkyl acids and their precursors in indoor air sampled in children′s bedrooms[J].Environmental Pollution,222:423-432
Yang L P,Tian S Y,Zhu L Y,et al.2012.Bioaccumulation and distribution of perfloroalkyl acids in seafood products from Bohai Bay,China[J].Environmental Toxicology and Chemistry,31(9):1972-1979
Yao Y,Zhao Y,Sun H,et al.2018.Per- and polyfluoroalkyl substances (PFASs) in indoor air and dust from homes and various microenvironments in china:implications for human exposure[J].Environmental Science & Technology,52(5):3156-3166
Yoo H,Guruge K S,Yamanaka N,et al.2009.Depuration kinetics and tissue disposition of PFOA and PFOS in white leghorn chickens (Gallus gallus) administered by subcutaneous implantation[J].Ecotoxicology & Environmental Safety,72(1):26-36
Yu Y,Xu D,Lu M,et al.2015.QuEChERs combined with online interference trapping LC-MS/MS method for the simultaneous determination of 20 polyfluoroalkane substances in dietary milk[J].Journal of Agricultural and Food Chemistry,63(16):4087-4095
Zhang T,Sun H W,Lin Y,et al.2011.Perfluorinated compounds in human blood,water,edible freshwater fish,and seafood in China:Daily intake and regional differences in human exposures [J].Journal of Agricultural and Food Chemistry,59(20):11168-11176
Zhang T,Sun H W,Wu Q,et al.2010.Perfluorochemicals in meat,eggs and indoor dust in China:Assessment of sources and pathways of human exposure to perfluorochemicals[J].Environmental Science & Technology,44(9):3572-3579
Zhao S Y,Fang S H,Zhu L Y,et al.2014.Mutual impacts of wheat (Triticum aestivum L.) and earthworms (Eisenia fetida) on the bioavailability of perfluoroalkyl substances (PFASs) in soil[J].Environmental pollution (Barking,Essex:1987),184:495-501
Zhao Y G,Wan H T,Law A,et al.2011.Risk assessment for human consumption of perfluorinated compound-contaminated freshwater and marine fish from Hong Kong and Xiamen[J].Chemosphere,85(2):277-283
Zhang H,Vestergren R,Wang T,et al.2017.Geographical differences in dietary exposure to perfluoroalkyl acids between manufacturing and application regions in China[J].Environmental Science & Technology,51(10):5747-5755
赵立杰,周萌,任新豪,等.2012.全氟辛烷磺酸和全氟辛烷羧酸在天津大黄堡湿地地区鱼体和蔬菜中的分布研究[J].农业环境科学学报,31(12):2321-2327
Eriksson U,Karrman A,Rotander A,et al.2013.Perfluoroalkyl substances (PFASs) in food and water from Faroe Islands[J].Environ Sci Pollut Res Int,20(11):7940-7948
European Food Safety Authority (EFSA).2008.Perfluorooctane sulfonate (PFOS),perfluorooctanoic acid (PFOA) and their salts scientific opinion of the panel on contaminants in the food chain[J].EFSA Journal,6(7):653:1-131
Fang S H,Chen X W,Zhao S Y,et al.2014.Trophic magnification and isomer fractionation of perfluoroalkyl substances in the food web of Taihu Lake,China[J].Environmental Science & Technology,48(4):2173-2182
Fuentes S,Vicens P,Colomina M,et al.2007.Behavioral effects in adult mice exposed to perfluorooctane sulfonate (PFOS) [J].Toxicology,242(1/3):123-129
Gebbink W A,Letcher R J.2012.Comparative tissue and body compartment accumulation and maternal transfer to eggs of perfluoroalkyl sulfonates and carboxylates in Great Lakes herring gulls[J].Environmental Pollution,162:40-47
Gebbink W A,Van Asseldonk L,Van Leeuwen S P J.2017.Presence of emerging per- and polyfluoroalkyl substances (PFASs) in river and drinking water near a fluorochemical production plant in the Netherlands[J].Environmental Science & Technology,51(19):11057-11065
Giesy J P,Kannan K.2001.Global distribution of perfluorooctane sulfonate in wildlife[J].Environmental Science & Technology,35(7):1339-1342
Gulkowska A,Jiang Q T,So M K,et al.2006.Persistent perfluorinated acids in seafood collected from two cities of China [J].Environmental Science & Technology,40(12):3736-3741
Holmstrom K E,Berger U.2008.Tissue distribution of perfluorinated surfactants in common guillemot (Uria aalge) from the Baltic Sea[J].Environmental Science & Technology,42(16):5879-5884
Heydebreck F,Tang J,Xie Z,et al.2016.Emissions of per- and polyfluoroalkyl substances in a textile manufacturing plant in china and their relevance for workers′ exposure[J].Environmental Science & Technology,50(19):10386-10396
Jin H,Zhang Y,Zhu L,et al.2015.Isomer profiles of perfluoroalkyl substances in water and soil surrounding a Chinese Fluorochemical Manufacturing Park[J].Environmental Science & Technology,49(8):4946-4954
Kleszczynski K,Gardzielewski P,Mulkiewicz E,et al.2007.Analysis of structure-cytotoxicity in vitro relationship (SAR) for perfluorinated carboxylic acids [J].Toxicology in Vitro,21(6):1206-1211
Lau C,Anitole K,Hodes C,et al.2007.Perfluoroalkyl acids:A review of monitoring and toxicological findings[J].Toxicological Sciences,99(2):366-394
柳思帆,王铁宇,薛科社,等.2017.北京水源地鱼体全氟化合物的暴露水平及其健康风险[J].生态毒理学报,12(1):111-118
罗超.2014.福建省大米中全氟烷基化合物污染水平调查[D].厦门:集美大学
Lofstrand K,Jorundsdottir H,Tomy G,et al.2008.Spatial trends of polyfluorinated compounds in guillemot (Uria aalge) eggs from North-Western Europe[J].Chemosphere,72(10):1475-1480
Martin J W,Mabury S A,Solomon K R,et al.2003a.Bioconcentration and tissue distribution of perfluorinated acids in rainbow trout (Oncorhynchus mykiss)[J].Environmental Toxicology and Chemistry,22(1):196-204
Martin J W,Mabury S A,Solomon K R,et al.2003b.Dietary accumulation of perfluorinated acids in juvenile rainbow trout (Oncorhynchus mykiss)[J].Environmental Toxicology & Chemistry,22(1):189-195
Meesters R J W,Schr?der H F.2004.Perfluorooctane sulfonate - a quite mobile anionic anthropogenic surfactant,ubiquitously found in the environment[J].Water Science and Technology,50(5):235-242
Poothong S,Thomsen C,Padilla-Sanchez J A,et al.2017.Distribution of novel and well-known poly- and perfluoroalkyl substances (PFASs) in human serum,plasma,and whole blood[J].Environmental Science & Technology,51(22):13388-13396
Powley C R,George S W,Ryan T W,et al.2005.Matrix effect-free analytical methods for determination of perfluorinated carboxylic acids in environmental matrixes[J].Analytical Chemistry,77(19):6353-6358
Shan G,Wang Z,Zhou L,et al.2016.Impacts of daily intakes on the isomeric profiles of perfluoroalkyl substances (PFASs) in human serum[J].Environment International,89-90:62-70
Shi Y L,Pan Y Y,Wang J M,et al.2012.Distribution of perfluorinated compounds in water,sediment,biota and floating plants in Baiyangdian Lake,China[J].Journal of Environmental Monitoring,14(2):636-642
Taniyasu S,Kannan K,Horii Y,et al.2003.A survey of perfluorooctane sulfonate and related perfluorinated organic compounds in water,fish,birds,and humans from Japan[J].Environmental Science & Technology,37(12):2634-2639
US-EPA.2006.PFOA Stewardship Program[OL].2006-10-31.http://www.epa.gov/oppt/pfoa/pubs/stewardship/pfoastewardshipbasics.html
Wang J,Shi Y,Pan Y,et al.2010a.Perfluorinated compounds in milk,milk powder and yoghurt purchased from markets in China[J].Chinese Science Bulletin,55(11):1020-1025
Wang J,Shi Y,Pan Y,et al.2010b.Perfluorooctane sulfonate (PFOS) and other fluorochemicals in viscera and muscle of farmed pigs and chickens in Beijing,China[J].Chinese Science Bulletin,55(31):3550-3555
Wang Y,Yeung L,Yamashita N,et al.2008.Perfluorooctane sulfonate (PFOS) and related fluorochemicals in chicken egg in China[J].Chinese Science Bulletin,53(4):501-507
Winkens K,Koponen J,Schuster J,et al.2017.Perfluoroalkyl acids and their precursors in indoor air sampled in children′s bedrooms[J].Environmental Pollution,222:423-432
Yang L P,Tian S Y,Zhu L Y,et al.2012.Bioaccumulation and distribution of perfloroalkyl acids in seafood products from Bohai Bay,China[J].Environmental Toxicology and Chemistry,31(9):1972-1979
Yao Y,Zhao Y,Sun H,et al.2018.Per- and polyfluoroalkyl substances (PFASs) in indoor air and dust from homes and various microenvironments in china:implications for human exposure[J].Environmental Science & Technology,52(5):3156-3166
Yoo H,Guruge K S,Yamanaka N,et al.2009.Depuration kinetics and tissue disposition of PFOA and PFOS in white leghorn chickens (Gallus gallus) administered by subcutaneous implantation[J].Ecotoxicology & Environmental Safety,72(1):26-36
Yu Y,Xu D,Lu M,et al.2015.QuEChERs combined with online interference trapping LC-MS/MS method for the simultaneous determination of 20 polyfluoroalkane substances in dietary milk[J].Journal of Agricultural and Food Chemistry,63(16):4087-4095
Zhang T,Sun H W,Lin Y,et al.2011.Perfluorinated compounds in human blood,water,edible freshwater fish,and seafood in China:Daily intake and regional differences in human exposures [J].Journal of Agricultural and Food Chemistry,59(20):11168-11176
Zhang T,Sun H W,Wu Q,et al.2010.Perfluorochemicals in meat,eggs and indoor dust in China:Assessment of sources and pathways of human exposure to perfluorochemicals[J].Environmental Science & Technology,44(9):3572-3579
Zhao S Y,Fang S H,Zhu L Y,et al.2014.Mutual impacts of wheat (Triticum aestivum L.) and earthworms (Eisenia fetida) on the bioavailability of perfluoroalkyl substances (PFASs) in soil[J].Environmental pollution (Barking,Essex:1987),184:495-501
Zhao Y G,Wan H T,Law A,et al.2011.Risk assessment for human consumption of perfluorinated compound-contaminated freshwater and marine fish from Hong Kong and Xiamen[J].Chemosphere,85(2):277-283
Zhang H,Vestergren R,Wang T,et al.2017.Geographical differences in dietary exposure to perfluoroalkyl acids between manufacturing and application regions in China[J].Environmental Science & Technology,51(10):5747-5755
赵立杰,周萌,任新豪,等.2012.全氟辛烷磺酸和全氟辛烷羧酸在天津大黄堡湿地地区鱼体和蔬菜中的分布研究[J].农业环境科学学报,31(12):2321-2327