广州市售水产品中全氟烷基化合物的污染特征和安全风险评价
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摘要
为调查广州市售水产品中全氟烷基化合物(perflurorinated alkylated substances,PFASs)的污染特征,采集鱼类、甲壳类和头足类等6类254个样品,采用超高效液相色谱串联质谱法测定23种PFASs的含量.不同种类样品的PFASs总检出率为93. 5%～100%,鱼类和甲壳类的含量较高.鱼类中检出了13种PFASs组分,但鲍鱼仅检出6种,种类差异明显.全氟辛烷磺酸(PFOS)和全氟辛烷羧酸(PFOA)的检出率最高,分别为76. 8%和75. 6%,为PFASs的特征污染组分. PFOS的含量为0. 19～192. 27μg·kg~(-1),明显高于其它组分,污染贡献率达35. 15%.与鱼类、甲壳类、头足类和加工制品中PFOS的污染贡献率最高不同,海珍品中污染贡献率最高的是全氟丁酸(PFBA),样品组分污染特征表现出明显的种类差异性.风险评价结果表明,广州市售水产品中PFOA和PFOS对人的潜在健康风险低.
To investigate the contamination characteristics of PFASs in aquatic products,254 samples belonging to 6 species,including fishes,crustaceans,cephalopods,etc.,were collected from Guangzhou,and 23 PFASs were determined by UPLC-MS/MS. The total detection rates of the various sample species ranged from 93. 5% to 100%,and the concentrations of PFASs were relatively higher in the fishes and crustaceans. 13 PFAS components were detected in the fish samples,but only 6 PFAS components were detected in haliotis samples,and obvious differences were observed among the different species sampled. PFOA and PFOS were the predominant pollutants,with detection rates of 75. 6% and 76. 8%. The concentrations of PFOS were in the range of 0. 19-192. 27 μg·kg~(-1),which were obviously higher than those of the other PFAS components,and their total contamination contribution factor reached the highest percentage of 35. 15%. PFOS was a major contributing factor to the PFAS contamination of fishes,crustaceans,siphonopods,and processed products; however,the predominant pollutant in Haliotis samples was PFBA. The results of the risk assessment indicated that the concentrations of PFOA and PFOS would not give rise to timely harm to the consumers.
To investigate the contamination characteristics of PFASs in aquatic products,254 samples belonging to 6 species,including fishes,crustaceans,cephalopods,etc.,were collected from Guangzhou,and 23 PFASs were determined by UPLC-MS/MS. The total detection rates of the various sample species ranged from 93. 5% to 100%,and the concentrations of PFASs were relatively higher in the fishes and crustaceans. 13 PFAS components were detected in the fish samples,but only 6 PFAS components were detected in haliotis samples,and obvious differences were observed among the different species sampled. PFOA and PFOS were the predominant pollutants,with detection rates of 75. 6% and 76. 8%. The concentrations of PFOS were in the range of 0. 19-192. 27 μg·kg~(-1),which were obviously higher than those of the other PFAS components,and their total contamination contribution factor reached the highest percentage of 35. 15%. PFOS was a major contributing factor to the PFAS contamination of fishes,crustaceans,siphonopods,and processed products; however,the predominant pollutant in Haliotis samples was PFBA. The results of the risk assessment indicated that the concentrations of PFOA and PFOS would not give rise to timely harm to the consumers.
引文
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[10]王超,吕怡兵,陈海君,等.固相萃取-液相色谱-串联质谱法同时测定水中14种短链和长链全氟化合物[J].色谱,2014,32(9):919-925.Wang C,Lv Y B,Chen H J,et al. Simultaneous analysis of 14short-and long-chain perfluorinated compounds in water by liquid chromatography-tandem mass spectrometry using solid phase extraction[J]. Chinese Journal of Chromatography,2014,32(9):919-925.
[11]李法松,倪卉,黄涵宇,等.安徽省部分城市土壤中全氟化合物空间分布及来源解析[J].环境科学,2017,38(1):327-332.Li F S,Ni H,Huang H Y,et al. Spatial distribution and source of perfluorinated compounds in urban soil from part of cities in Anhui province,China[J]. Environmental Science,2017,38(1):327-332.
[12]刘庆,贺德春,许振成,等.液相色谱-串联质谱法测定水体、沉积物及土壤中全氟化合物[J].中国环境监测,2014,30(4):134-139.Liu Q,Tang D C,Xu Z C,et al. Analysis of Polyfluoroalkyl chemicals in water,sediments and soil by liquid chromatographytandem mass spectrometry[J]. Environmental Monitoring in China,2010,30(4):134-139.
[13]王懿,孔德洋,单正军,等.加速溶剂萃取-固相萃取净化-超高效液相色谱串联质谱法测定土壤中11种全氟化合物[J].环境化学,2012,31(1):113-119.Wang Y,Kong D X,Shan Z J,et al. Analysis of perfluorinated compounds in soil by accelerated solvent extraction combined with ultra performance liquid chromatographytandem mass spectrometry[J]. Environmental Chemisty,2012,31(1):113-119.
[14]孟晶,王铁宇,王佩,等.淮河流域土壤中全氟化合物的空间分布及组成特征[J].环境科学,2013,34(8):3188-3194.Meng J,Wang T Y,Yang P,et al. Spatial distribution and composition of perfluorinated compounds in soils around the Huaihe River[J]. Environmental Science,2013,34(8):3188-3194.
[15]李静,张鸿,柴之芳,等.分散固相萃取结合HPLC-MS/MS检测鸡蛋中16种全氟化合物[J].分析测试学报,2014,33(10):1109-1115.Li J, Zhang H, Chai Z F, et al. Determination of sixteen perfluorinated compounds in egg by high performance liquid chromatography-tandem mass spectrometry combined with dispersive solid phase extraction[J]. Journal of Instrumental Analysis,2014,33(10):1109-1115.
[16]何建丽,彭涛,谢洁,等.高效液相色谱-串联质谱法测定动物肝脏中20种全氟烷基类化合物[J].分析化学,2015,43(1):40-48.He J L,Peng T,Xie J,et al. Development of a Qu ECh ERs method for determination of 20perfluorinated compounds in animal liver by HPLC-MS/MS[J]. Chinese Journal of Analytical Chemistry,2015,43(1):40-48.
[17]郭萌萌,吴海燕,李兆新,等.超快速液相色谱-串联质谱法检测水产品中23种全氟烷基化合物[J].分析化学,2013,41(9):1322-1327.Guo M M, Wu H Y, Li Z X, et al. Determination of 23perfluorinated alkyl substances in Fishery products by ultra fast liquid chromatography tandem mass spectrometry[J]. Chinese Journal of Analytical Chemistry,2013,41(9):1322-1327.
[18]郭萌萌,吴海燕,卢立娜,等.杂质延迟-液相色谱-四极杆/离子阱复合质谱测定水产加工食品中23种全氟烷基化合物[J].分析化学,2015,43(8):1105-1112.Guo M M,Wu H Y,Lu L N,et al. Simultaneous identification and detection of 23 perfluorinated alkyl substances in processed aquatic products by impurity delay using liquid chromatography coupled with quadrupole/linear ion trap mass spectrometry[J].Chinese Journal of Analytical Chemistry,2015,43(8):1105-1112.
[19] Berger U,Glynn A,Holmstrom K E,et al. Fish consumption as a source of human exposure to perfluorinated alkyl substances in Sweden-Analysis of edible fish from Lake Vattern and the Baltic Sea[J]. Chemosphere,2009,76(6):799-804.
[20] Domingo J L,Ericson-Jogeten I,PerellóG,et al. Human exposure to perfluorinated compounds in Catalonia, Spain:contribution of drinking water and fish and shellfish[J]. Journal of Agriculture and Food Chemistry,2012,60(17):4408-4415.
[21] Schuetze A,Heberer T,Effkemann S,et al. Occurrence and assessment of perfluorinated chemicals in wild fish from Northern Germany[J]. Chemosphere,2010,78(6):647-652.
[22] Nania V, Pellegrini G E, Fabrizi L, et al. Monitoring of perfluorinated compounds in edible fish from the Mediterranean Sea[J]. Food Chemistry,2009,115(3):951-957.
[23] Gulkowska A, Jiang Q T, So M K, et al. Persistent perfluorinated acids in seafood collected from two cities of China[J]. Environmental Science&Technology,2006,40(12):3736-3741.
[24] Wu Y N,Wang L X,Li J G,et al. Perfluorinated compounds in seafood from coastal areas in China[J]. Environment International,2012,42:67-71.
[25] Zhao Y G,Wan H T,Wong M H,et al. Partitioning behavior of perfluorinated compounds between sediment and biota in the Pearl River Delta of South China[J]. Marine Pollution Bulletin,2014,83(1):148-154.
[26] Pan C G,Yu K F,Wang Y H,et al. Species-specific profiles and risk assessment of perfluoroalkyl substances in coral reef fishes from the South China Sea[J]. Chemosphere,2018,191:450-457.
[27]张明,唐访良,俞雅雲,等.杭州地区城区降雪中全氟化合物的污染特征[J].环境科学,2017,38(8):3185-3191.Zhang M,Tang F L,Yu Y Y,et al. Perfluorinated compounds in snow from downtown Hangzhou,China[J]. Environmental Science,2018,38(8):3185-3191.
[28]齐彦杰,周珍,史亚利,等.北京市市售鸡蛋和鸭蛋中全氟化合物的污染水平研究[J].环境科学,2013,34(1):244-250.Qi Y J, Zhou Z, Shi Y L, et al. Pollution levels of perfluorochemicals in chicken eggs and duck eggs from the markets in Beijing[J]. Environmental Science,2013,34(1):244-250.
[29]岳冬冬,王鲁民,方海,等.中国城乡居民水产品消费量与收入差距关系研究[J].渔业信息与战略,2018,33(1):1-8.Yue D D,Wang L M,Fang H,et al. On the relationship between aquatic products consumption and income gap of urban and rural households in China[J]. Fishery Information&Strategy,2018,33(1):1-8.
[2]郑建国,刘葳,张子豪,等.高效液相色谱-串联质谱法测定纺织品中16种全氟烷酸类化合物[J].分析测试学报,2016,35(2):213-218.Zheng J G,Liu W,Zhang Z H,et al. Determination of 16perfluoroalkyl acids in textiles by HPLC-MS/MS[J]. Journal of Instrumental Analysis,2016,35(2):213-218.
[3]陈笑梅,刘慧婷,谢维斌,等.食品接触材料中全氟烷基磺酸类化合物的HPLC-MS/MS测定[J].食品科学,2010,31(8):174-176.Chen X M, Liu H T, Xie W B, et al. HPLC-MS/MS determination of perfluoroalkane sulfonates in food contact materials[J]. Food Science,2010,31(8):174-176.
[4] Wei Y H,Dai J Y,Liu M,et al. Estrogen-like properties of perfluorooctanoic acid as revealed by expressing hepatic estrogenresponsive genes in rare minnows(Gobiocypris rarus)[J].Environmental Toxicology Chemistry,2007,26(11):2440-2447.
[5] Johansson N,Fredriksson A,Eriksson P. Neonatal exposure to perfluorooctane sulfonate(PFOS)and perfluorooctanoic acid(PFOA)causes neurobehavioural defects in adult mice[J].NeuroToxicology,2008,29(1):160-169.
[6] Zheng L,Dong G H,Jin Y H,et al. Immunotoxic changes associated with a 7-day oral exposure to perfluorooctanesulfonate(PFOS)in adult male C57BL/6 mice[J]. Archives of Toxicology,2009,83(7):679-689.
[7]崔晓宇,张鸿,罗骥,等.深圳地区全氟辛烷磺酸的环境多介质迁移和归趋行为研究[J].环境科学,2016,37(8):3001-3006.Cui X Y,Zhang H,Luo J,et al. Simulation of multimedia transfer and fate of perfluorooctane sulfonate(PFOS)in Shenzhen Region[J]. Environmental Science,2016,37(8):3001-3006.
[8] European Food Safety Authority. Results of the monitoring of perfluoroalkylated substances in food in the period 2000-2009[J]. EFSA Journal,2011,9(2):2016.
[9]杨永亮,路国慧,杨伟贤,等.沈阳地区水环境和生物样品中全氟化合物的污染分布特征[J].环境科学学报,2010,30(10):2097-2107.Yang Y L,Luo G H,Yang W X,et al. Levels and distribution of perfluorinated compounds in water and biological samples from the Shenyang area[J]. Acta Scientiae Circumstantiae,2010,30(10):2097-2107.
[10]王超,吕怡兵,陈海君,等.固相萃取-液相色谱-串联质谱法同时测定水中14种短链和长链全氟化合物[J].色谱,2014,32(9):919-925.Wang C,Lv Y B,Chen H J,et al. Simultaneous analysis of 14short-and long-chain perfluorinated compounds in water by liquid chromatography-tandem mass spectrometry using solid phase extraction[J]. Chinese Journal of Chromatography,2014,32(9):919-925.
[11]李法松,倪卉,黄涵宇,等.安徽省部分城市土壤中全氟化合物空间分布及来源解析[J].环境科学,2017,38(1):327-332.Li F S,Ni H,Huang H Y,et al. Spatial distribution and source of perfluorinated compounds in urban soil from part of cities in Anhui province,China[J]. Environmental Science,2017,38(1):327-332.
[12]刘庆,贺德春,许振成,等.液相色谱-串联质谱法测定水体、沉积物及土壤中全氟化合物[J].中国环境监测,2014,30(4):134-139.Liu Q,Tang D C,Xu Z C,et al. Analysis of Polyfluoroalkyl chemicals in water,sediments and soil by liquid chromatographytandem mass spectrometry[J]. Environmental Monitoring in China,2010,30(4):134-139.
[13]王懿,孔德洋,单正军,等.加速溶剂萃取-固相萃取净化-超高效液相色谱串联质谱法测定土壤中11种全氟化合物[J].环境化学,2012,31(1):113-119.Wang Y,Kong D X,Shan Z J,et al. Analysis of perfluorinated compounds in soil by accelerated solvent extraction combined with ultra performance liquid chromatographytandem mass spectrometry[J]. Environmental Chemisty,2012,31(1):113-119.
[14]孟晶,王铁宇,王佩,等.淮河流域土壤中全氟化合物的空间分布及组成特征[J].环境科学,2013,34(8):3188-3194.Meng J,Wang T Y,Yang P,et al. Spatial distribution and composition of perfluorinated compounds in soils around the Huaihe River[J]. Environmental Science,2013,34(8):3188-3194.
[15]李静,张鸿,柴之芳,等.分散固相萃取结合HPLC-MS/MS检测鸡蛋中16种全氟化合物[J].分析测试学报,2014,33(10):1109-1115.Li J, Zhang H, Chai Z F, et al. Determination of sixteen perfluorinated compounds in egg by high performance liquid chromatography-tandem mass spectrometry combined with dispersive solid phase extraction[J]. Journal of Instrumental Analysis,2014,33(10):1109-1115.
[16]何建丽,彭涛,谢洁,等.高效液相色谱-串联质谱法测定动物肝脏中20种全氟烷基类化合物[J].分析化学,2015,43(1):40-48.He J L,Peng T,Xie J,et al. Development of a Qu ECh ERs method for determination of 20perfluorinated compounds in animal liver by HPLC-MS/MS[J]. Chinese Journal of Analytical Chemistry,2015,43(1):40-48.
[17]郭萌萌,吴海燕,李兆新,等.超快速液相色谱-串联质谱法检测水产品中23种全氟烷基化合物[J].分析化学,2013,41(9):1322-1327.Guo M M, Wu H Y, Li Z X, et al. Determination of 23perfluorinated alkyl substances in Fishery products by ultra fast liquid chromatography tandem mass spectrometry[J]. Chinese Journal of Analytical Chemistry,2013,41(9):1322-1327.
[18]郭萌萌,吴海燕,卢立娜,等.杂质延迟-液相色谱-四极杆/离子阱复合质谱测定水产加工食品中23种全氟烷基化合物[J].分析化学,2015,43(8):1105-1112.Guo M M,Wu H Y,Lu L N,et al. Simultaneous identification and detection of 23 perfluorinated alkyl substances in processed aquatic products by impurity delay using liquid chromatography coupled with quadrupole/linear ion trap mass spectrometry[J].Chinese Journal of Analytical Chemistry,2015,43(8):1105-1112.
[19] Berger U,Glynn A,Holmstrom K E,et al. Fish consumption as a source of human exposure to perfluorinated alkyl substances in Sweden-Analysis of edible fish from Lake Vattern and the Baltic Sea[J]. Chemosphere,2009,76(6):799-804.
[20] Domingo J L,Ericson-Jogeten I,PerellóG,et al. Human exposure to perfluorinated compounds in Catalonia, Spain:contribution of drinking water and fish and shellfish[J]. Journal of Agriculture and Food Chemistry,2012,60(17):4408-4415.
[21] Schuetze A,Heberer T,Effkemann S,et al. Occurrence and assessment of perfluorinated chemicals in wild fish from Northern Germany[J]. Chemosphere,2010,78(6):647-652.
[22] Nania V, Pellegrini G E, Fabrizi L, et al. Monitoring of perfluorinated compounds in edible fish from the Mediterranean Sea[J]. Food Chemistry,2009,115(3):951-957.
[23] Gulkowska A, Jiang Q T, So M K, et al. Persistent perfluorinated acids in seafood collected from two cities of China[J]. Environmental Science&Technology,2006,40(12):3736-3741.
[24] Wu Y N,Wang L X,Li J G,et al. Perfluorinated compounds in seafood from coastal areas in China[J]. Environment International,2012,42:67-71.
[25] Zhao Y G,Wan H T,Wong M H,et al. Partitioning behavior of perfluorinated compounds between sediment and biota in the Pearl River Delta of South China[J]. Marine Pollution Bulletin,2014,83(1):148-154.
[26] Pan C G,Yu K F,Wang Y H,et al. Species-specific profiles and risk assessment of perfluoroalkyl substances in coral reef fishes from the South China Sea[J]. Chemosphere,2018,191:450-457.
[27]张明,唐访良,俞雅雲,等.杭州地区城区降雪中全氟化合物的污染特征[J].环境科学,2017,38(8):3185-3191.Zhang M,Tang F L,Yu Y Y,et al. Perfluorinated compounds in snow from downtown Hangzhou,China[J]. Environmental Science,2018,38(8):3185-3191.
[28]齐彦杰,周珍,史亚利,等.北京市市售鸡蛋和鸭蛋中全氟化合物的污染水平研究[J].环境科学,2013,34(1):244-250.Qi Y J, Zhou Z, Shi Y L, et al. Pollution levels of perfluorochemicals in chicken eggs and duck eggs from the markets in Beijing[J]. Environmental Science,2013,34(1):244-250.
[29]岳冬冬,王鲁民,方海,等.中国城乡居民水产品消费量与收入差距关系研究[J].渔业信息与战略,2018,33(1):1-8.Yue D D,Wang L M,Fang H,et al. On the relationship between aquatic products consumption and income gap of urban and rural households in China[J]. Fishery Information&Strategy,2018,33(1):1-8.