食品接触材料中全氟化合物的迁移规律研究
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摘要
目的研究全氟化合物从食品接触材料到食品模拟物中的迁移规律。方法根据全氟化合物制品在日常生活中的使用情况,选择4个品牌的纸杯和3个品牌的包装袋进行了试验,以全氟辛酸、全氟辛烷磺酸等为研究对象,参考食品接触材料及制品迁移试验通则的具体要求,采用不同食品模拟物、不同操作方式、不同保存时间和温度等因素考察对全氟新烷磺酸、全氟辛酸的迁移量和迁移规律的影响。目标化合物通过C_(18)色谱柱进行分离,以乙腈-5 mmol/L的乙酸铵为流动相进行梯度洗脱;流速0.2 mL/min;柱温为30℃;进样量1μL,由三重四级杆质谱进行定性和定量分析。结果数据显示在模拟物为食用油时PFOA的迁移量是最大的,超过0.01 ng/cm~2;其他情况PFOA的溶出量都低于0.002 ng/cm~2; PFOS的溶出量均较少,低于0.002 ng/cm~2。结论初步得到食品接触材料中典型全氟化合物的迁移规律基础数据,说明无论是何种品牌的纸杯或是包装袋,接触食物均会产生PFOA和PFOS的微量溶出,经过膳食暴露可能会引起健康危害。
Objective To study the migration of perfluorinated compounds from food contact materials to food simulants. Methods According to the use of perfluorochemical products in daily life, 4 brands of paper cups and 3 brands of package bags were selected for testing. Perfluorooctanoic acid and perfluorooctane sulfonic acid were taken as the research objects, and the specific requirements of the general rules for the migration of food contact materials and products were referred. The effects of different food simulants, different operation methods, different storage time and temperature on the migration quantity and migration rule of perfluorooctanoic acid and perfluorooctanoic acid were investigated. The target compounds were separated by C_(18) column and eluted with acetonitrile-5 mmol/L ammonium acetate as the mobile phase, the flow rate was 0.2 mL/min, the column temperature was 30 ℃, the injection volume was 1 μL, and the triple quadrupole mass spectrometry was performed for qualitative and quantitative analysis. Results The data showed that the migration of PFOA was the most when the simulant was edible oil, exceeding 0.01 ng/cm~2. In other cases, the leaching amount of PFOA was less than 0.002 ng/cm~2. The leaching amount of PFOS was less than 0.002 ng/cm~2. Conclusion This paper preliminarily obtain the basic data of the migration law of typical perfluorinated compounds in food contact materials, indicating that no matter what brand of paper cups or packaging bags, PFOA and PFOS microdissolution could be generated after food contact, and the dietary exposure might cause health hazards.
Objective To study the migration of perfluorinated compounds from food contact materials to food simulants. Methods According to the use of perfluorochemical products in daily life, 4 brands of paper cups and 3 brands of package bags were selected for testing. Perfluorooctanoic acid and perfluorooctane sulfonic acid were taken as the research objects, and the specific requirements of the general rules for the migration of food contact materials and products were referred. The effects of different food simulants, different operation methods, different storage time and temperature on the migration quantity and migration rule of perfluorooctanoic acid and perfluorooctanoic acid were investigated. The target compounds were separated by C_(18) column and eluted with acetonitrile-5 mmol/L ammonium acetate as the mobile phase, the flow rate was 0.2 mL/min, the column temperature was 30 ℃, the injection volume was 1 μL, and the triple quadrupole mass spectrometry was performed for qualitative and quantitative analysis. Results The data showed that the migration of PFOA was the most when the simulant was edible oil, exceeding 0.01 ng/cm~2. In other cases, the leaching amount of PFOA was less than 0.002 ng/cm~2. The leaching amount of PFOS was less than 0.002 ng/cm~2. Conclusion This paper preliminarily obtain the basic data of the migration law of typical perfluorinated compounds in food contact materials, indicating that no matter what brand of paper cups or packaging bags, PFOA and PFOS microdissolution could be generated after food contact, and the dietary exposure might cause health hazards.
引文
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[8]路国慧,沈亚婷,何俊,等.高效液相色谱-串联质谱法测定黄河河口段水中全氟化合物的初步研究[J].岩矿测试,2012,31(1):147-151.Lu GH,Shen YT,He J,et al.Preliminary study on determination of perfluorinated compounds in water of the Yellow river estuary by high performance liquid chromatography-tandem mass spectrometry[J].Rock Ore Test,2012,31(1):147-151.
[9]Zhao RS,Wang X,Wang X,et al.Using bamboo charcoal as solid-phase extraction adsorbent for the ultratrace-level determination of perfluorooctanoic acid in water samples by HPLC-mass spectrometry[J].Anal Bioanal Chem,2008,390(6):1671-1676.
[10]王雨昕,李敬光,赵云峰,等.生物基质中全氟辛酸与全氟辛烷磺酸及其前体化合物的超高效液相色谱-串联质谱法研究[J].分析化学,2011,39(8):1134-1140.Wang YX,Li JG,Zhao YF,et al.Study on perfluorooctanoic acid and perfluorooctane sulfonic acid and their precursors in biological matrix by ultra-high performance liquid chromatography-tandem mass spectrometry[J].Anal Chem,2011,39(8):1134-1140.
[11]程家辉,李鑫,程红艳,等.近岸海水中全氟化合物的液相色谱-离子阱质谱法测定.[J].环境化学,2012,31(6):896-901.Cheng JH,Li X,Cheng HY,et al.Determination of perfluorinated compounds in offshore seawater by liquid chromatography-ion trap mass spectrometry[J].Environ Chem,2012,31(6):896-901.
[12]张晓丽,刘崇华,冼燕萍,等.液相色谱-串联质谱法测定纺织品中7种全氟有机物[J].2010,29(12):1182-1185.Zhang XL,Liu CH,Xian YP,et al.Determination of 7 perfluorinated organics in textiles by liquid chromatography-tandem mass spectrometry[J].2010,29(12):1182-1185.
[13]孔德洋,王懿,王娜,等.超高效液相色谱串联质谱法检测鱼体中的全氟化合物[J].环境化学,2012,31(5):743-747.Kong DY,Wang Y,Wang N,et al.Detection of perfluorinated compounds in fish by HPLC/MS[J].Environ Chem,2012,31(5):743-747.
[14]张岩,庞坤,吕品,等.液相色谱-串联质谱法测定食品用纸容器中全氟辛酸[J].食品科学,2012,33(22):207-209.Zhang Y,Pang K,Lv P,et al.Determination of perfluorooctanoic acid in food paper containers by liquid chromatography-tandem mass spectrometry[J].Food Sci,2012,33(22):207-209.
[15]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 YJ,Zhou Z,Shi YL,et al.Study on the pollution level of perfluorinated compounds in commercial eggs and duck eggs in Beijing[J].Environ Sci,2013,34(1):244-250.
[16]Boone JS,Guan B,Vigo C,et al.A method for the analysis of perfluorinated compounds in environmental and drinking waters and the determination of their lowest concentration minimal reporting levels[J].JChromatogr A,2014,1345:68-77.
[17]王杰明,王丽,冯玉静,等.液相色谱-质谱联用分析动物内脏和肌肉组织中的全氟化合物[J].食品科学,2010,(4):127-131.Wang JM,Wang L,Feng YJ,et al.Analysis of perfluorinated compounds in animal viscera and muscle tissues by liquid chromatography-mass spectrometry[J].Food Sci,2010,(4):127-131.
[18]Lashgari M,Lee HK.Determination of perfluorinated carboxylic acids in fish fillet by micro-solid phase extraction,followed by liquid chromatography-triple quadrupole mass spectrometry[J].J Chromatogr A,2014,1369:26-32.
[19]GB 31604.1-2015食品安全国家标准食品接触材料及制品迁移试验通则[S].GB 31604.1-2015 National food safety standard-General principles for the test of migration of food contact materials and products[S].
[2]Gebbink WA,Letcher RJ.Comparative tissue and body compartment accumulation and maternal transfer to eggs of perfluoroalkyl sulfonates and carboxylates in Great Lakes herring gulls[J].Environ Poll,2012,162:40-47.
[3]Perfluorooctane sulfonate(PFOS),perfluorooctanoic acid(PFOA)and their salts[Z].2008.
[4]Wu YN,Wang YX,Li JG,et al.Perfluorinated compounds in seafood from coastal areas in China[J].Environ Int,2012,42:67-71.
[5]武晓果,谢周清.南北极全氟化合物的含量、分布及迁移[J].极地研究,2009,21(3):197-210.Wu XG,Xie ZQ.Content,distribution and migration of perfluorinated compounds in arctic and antarctic[J].Polar Res,2009,21(3):197-210.
[6]王亚韡,蔡亚岐,江桂斌.斯德哥尔摩公约新增持久性有机污染物的一些研究进展[J].中国科学,2010,40(2):99-123.Wang YH,Cai YQ,Jiang GB.New in Stockholm convention on persistent organic pollutants(pops)some research progress[J].Sci China,2010,40(2):99-123.
[7]楼军,鲍宗必,吴晓晋,等.气相色谱-质谱联用法分析全氟酰氟[J].分析化学,2013,41(7):1086-1090.Lou J,Bao ZB,Wu XJ,et al.Gas chromatography-mass spectrometry analysis of perfluoroacyl fluoride[J].Anal Chem,2013,41(7):1086-1090.
[8]路国慧,沈亚婷,何俊,等.高效液相色谱-串联质谱法测定黄河河口段水中全氟化合物的初步研究[J].岩矿测试,2012,31(1):147-151.Lu GH,Shen YT,He J,et al.Preliminary study on determination of perfluorinated compounds in water of the Yellow river estuary by high performance liquid chromatography-tandem mass spectrometry[J].Rock Ore Test,2012,31(1):147-151.
[9]Zhao RS,Wang X,Wang X,et al.Using bamboo charcoal as solid-phase extraction adsorbent for the ultratrace-level determination of perfluorooctanoic acid in water samples by HPLC-mass spectrometry[J].Anal Bioanal Chem,2008,390(6):1671-1676.
[10]王雨昕,李敬光,赵云峰,等.生物基质中全氟辛酸与全氟辛烷磺酸及其前体化合物的超高效液相色谱-串联质谱法研究[J].分析化学,2011,39(8):1134-1140.Wang YX,Li JG,Zhao YF,et al.Study on perfluorooctanoic acid and perfluorooctane sulfonic acid and their precursors in biological matrix by ultra-high performance liquid chromatography-tandem mass spectrometry[J].Anal Chem,2011,39(8):1134-1140.
[11]程家辉,李鑫,程红艳,等.近岸海水中全氟化合物的液相色谱-离子阱质谱法测定.[J].环境化学,2012,31(6):896-901.Cheng JH,Li X,Cheng HY,et al.Determination of perfluorinated compounds in offshore seawater by liquid chromatography-ion trap mass spectrometry[J].Environ Chem,2012,31(6):896-901.
[12]张晓丽,刘崇华,冼燕萍,等.液相色谱-串联质谱法测定纺织品中7种全氟有机物[J].2010,29(12):1182-1185.Zhang XL,Liu CH,Xian YP,et al.Determination of 7 perfluorinated organics in textiles by liquid chromatography-tandem mass spectrometry[J].2010,29(12):1182-1185.
[13]孔德洋,王懿,王娜,等.超高效液相色谱串联质谱法检测鱼体中的全氟化合物[J].环境化学,2012,31(5):743-747.Kong DY,Wang Y,Wang N,et al.Detection of perfluorinated compounds in fish by HPLC/MS[J].Environ Chem,2012,31(5):743-747.
[14]张岩,庞坤,吕品,等.液相色谱-串联质谱法测定食品用纸容器中全氟辛酸[J].食品科学,2012,33(22):207-209.Zhang Y,Pang K,Lv P,et al.Determination of perfluorooctanoic acid in food paper containers by liquid chromatography-tandem mass spectrometry[J].Food Sci,2012,33(22):207-209.
[15]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 YJ,Zhou Z,Shi YL,et al.Study on the pollution level of perfluorinated compounds in commercial eggs and duck eggs in Beijing[J].Environ Sci,2013,34(1):244-250.
[16]Boone JS,Guan B,Vigo C,et al.A method for the analysis of perfluorinated compounds in environmental and drinking waters and the determination of their lowest concentration minimal reporting levels[J].JChromatogr A,2014,1345:68-77.
[17]王杰明,王丽,冯玉静,等.液相色谱-质谱联用分析动物内脏和肌肉组织中的全氟化合物[J].食品科学,2010,(4):127-131.Wang JM,Wang L,Feng YJ,et al.Analysis of perfluorinated compounds in animal viscera and muscle tissues by liquid chromatography-mass spectrometry[J].Food Sci,2010,(4):127-131.
[18]Lashgari M,Lee HK.Determination of perfluorinated carboxylic acids in fish fillet by micro-solid phase extraction,followed by liquid chromatography-triple quadrupole mass spectrometry[J].J Chromatogr A,2014,1369:26-32.
[19]GB 31604.1-2015食品安全国家标准食品接触材料及制品迁移试验通则[S].GB 31604.1-2015 National food safety standard-General principles for the test of migration of food contact materials and products[S].