固相萃取-超高效液相色谱-串联质谱法测定污水中16种全氟和多氟烷基化合物
Determination of 16 Perfluoroalkyl and Polyfluoroalkyl Substances in Wastewater by Solid Phase Extraction-Ultraperformance Liquid Chromatography-Tandem Mass Spectrometry
-
摘要: 建立了以固相萃取-超高效液相色谱-串联质谱同时测定污水中16种全氟和多氟烷基化合物（PFASs）的方法。样品经固相萃取柱富集浓缩，采用BEH-C18色谱柱（2.1 mm×100 mm，1.7 μm），以甲醇和5 mmol·L-1乙酸铵溶液（pH=9）为流动相梯度淋洗，负离子多反应监测模式进行定性和定量分析，内标法定量。16种PFASs在0.1～40 μg·L-1范围内线性关系良好，相关系数（r2）>0.99，目标物加标回收率为65.1%～129.0%，相对标准偏差（RSD）为0.8%～8.0%（n=6），方法检出限为0.012～4.00 ng·L-1。方法重现性好，灵敏度高。适用于污水中PFASs的定量测定。
-
关键词:
- 全氟和多氟烷基化合物 /
- 固相萃取-超高效液相色谱-串联质谱 /
- 污水
Abstract: A method for the simultaneous determination of 16 perfluoroalkyl and polyfluoroalkyl substances (PFASs) in wastewater by solid phase extraction-ultra performance liquid chromatography-tandem mass spectrometry was established. The sample was enriched and concentrated on a solid-phase extraction column with a BEH-C18 column (2.1 mm×100 mm, 1.7 μm), using methanol and 5 mmol·L-1ammonium acetate solution (pH=9) as mobile phases with gradient elution, and quantified in the negative ion multiple reaction monitoring mode with internal standard method. The linear range of the 16 PFASs was 0.1~40 μg·L-1 with the correlation coefficients (r2) greater than 0.99, the spiked recoveries were 65.1%~129.0%, the relative standard deviations (RSD) were 0.8%~8.0% (n=6), and the method limits of detection were 0.012~4.00 ng·L-1. The method has good reproducibility and high sensitivity. It is suitable for the quantitative determination of PFASs in wastewater. -
-
郝薛文, 李力, 王杰, 等. 全氟和多氟烷基化合物的环境风险评估研究现状、不确定性与趋势分析[J]. 环境科学, 2015, 36(8):3106-3118 Hao X W, Li L, Wang J, et al. Status quo, uncertainties and trends analysis of environmental risk assessment for PFASs[J]. Environmental Science, 2015, 36(8):3106-3118(in Chinese)
何鹏, 何春兰, 陈忠. 食品接触材料中全氟/多氟烷基化合物的监管及对其替代品的思考[J]. 食品安全质量检测学报, 2020, 11(4):1033-1039 He P, He C L, Chen Z. Regulatory requirements of per-and polyfluoroalkyl substances used in food contact materials and insights on their alternatives[J]. Journal of Food Safety & Quality, 2020, 11(4):1033-1039(in Chinese)
孔祥云, 王华, 陈虹, 等. 全氟化合物的环境污染与毒性研究[J]. 环境科学与技术, 2015, 38(S1):5-9 Kong X Y, Wang H, Chen H, et al. Concentrations of perfluorinated compounds in the environment and their toxicity[J]. Environmental Science & Technology, 2015, 38(S1):5-9(in Chinese)
宋涛, 鲍佳, 刘洋, 等. 市政污泥处理过程中全氟化合物浓度的变化趋势研究[J]. 环境与发展, 2020, 32(8):207-209 Song T, Bao J, Liu Y, et al. Study on the changing trend of the concentration of perfluorinated compounds in the process of municipal sludge treatment[J]. Environment and Development, 2020, 32(8):207-209(in Chinese)
张慧, 王世亮, 余杨. 乐安河河流水体典型全氟化合物的浓度及其前体物的污染贡献[J]. 环境科学, 2020, 41(7):3204-3211 Zhang H, Wang S L, Yu Y. Concentrations of typical perfluoroalkyl acids and contributions of their precursors in the water of the Le'an River in China[J]. Environmental Science, 2020, 41(7):3204-3211(in Chinese)
杨洪法, 史斌, 周云桥, 等. 中、韩滨海城市化区域水体全氟化合物的空间特征及生态风险[J]. 环境科学, 2020, 41(4):1607-1618 Yang H F, Shi B, Zhou Y Q, et al. Spatial characteristics and ecological risks of perfluoroalkyl substances in coastal urbanized areas of China and south Korea[J]. Environmental Science, 2020, 41(4):1607-1618(in Chinese)
杜国勇, 蒋小萍, 卓丽, 等. 长江流域重庆段水体中全氟化合物的污染特征及风险评价[J]. 生态环境学报, 2019, 28(11):2266-2272 Du G Y, Jiang X P, Zhuo L, et al. Distribution characteristics and risk assessment of perfluorinated compounds in surface water from Chongqing section of the Yangtze River[J]. Ecology and Environmental Sciences, 2019, 28(11):2266-2272(in Chinese)
崔文杰, 彭吉星, 谭志军, 等. 全氟烷基物质在胶州湾海水、沉积物及生物中污染特征[J]. 环境科学, 2019, 40(9):3990-3999 Cui W J, Peng J X, Tan Z J, et al. Pollution characteristics of perfluorinated alkyl substances (PFASs) in seawater, sediments, and biological samples from Jiaozhou Bay, China[J]. Environmental Science, 2019, 40(9):3990-3999(in Chinese)
高杰, 李文超, 李广贺, 等. 北京部分地区地下水中全氟化合物的污染水平初探[J]. 生态毒理学报, 2016, 11(2):355-363 Gao J, Li W C, Li G H, et al. Preliminary investigation on perfluorinated compounds in groundwater in some areas of Beijing, China[J]. Asian Journal of Ecotoxicology, 2016, 11(2):355-363(in Chinese)
方淑红, 朱和祥, 叶芝祥, 等. 成都市道路积尘中全氟化合物的污染特征及暴露风险评估[J]. 环境科学, 2019, 40(12):5265-5271 Fang S H, Zhu H X, Ye Z X, et al. Pollution characteristics and exposure risk assessment of perfluoroalkyl substances in road dust, Chengdu[J]. Environmental Science, 2019, 40(12):5265-5271(in Chinese)
杨朔, 陈辉伦, 盖楠, 等. 北京市大气颗粒物中全氟烷基化合物的粒径分布特征[J]. 岩矿测试, 2018, 37(5):549-557 Yang S, Chen H L, Gai N, et al. Particle size distribution of perfluoroalkyl substances in atmospheric particulate matter in Beijing[J]. Rock and Mineral Analysis, 2018, 37(5):549-557(in Chinese)
方祥光, 赵祯, 李军, 等. 中国典型城市和地区大气颗粒物中全氟烷基酸的污染分布特征[J]. 环境化学, 2018, 37(7):1445-1459 Fang X G, Zhao Z, Li J, et al. Concentrations and distribution of perfluoroalkyl acids in the atmospheric particles in typical cities and regions of China[J]. Environmental Chemistry, 2018, 37(7):1445-1459(in Chinese)
郭萌萌, 崔文杰, 刘晓玉, 等. 黄渤海区域水产品中全氟烷基物质的分布特征[J]. 中国环境科学, 2020, 40(8):3424-3432 Guo M M, Cui W J, Liu X Y, et al. Distribution of perfluoroalkyl substances in aquatic products in coastal and adjacent areas of the Yellow Sea and Bohai Sea, China[J]. China Environmental Science, 2020, 40(8):3424-3432(in Chinese)
高艳飞, 那广水, 高会, 等. 全氟烷基磺酸和全氟烷基羧酸在水生动物体内富集及毒性研究进展[J]. 环境与健康杂志, 2015, 32(10):930-934 Gao Y F, Na G S, Gao H, et al. Research progress on enrichment and toxicity of PFOS and PFOA in aquatic animals[J]. Journal of Environment and Health, 2015, 32(10):930-934(in Chinese)
孙玉珠, 李建宇, 武梦茹, 等. 动物性食品中全氟烷基物质的残留现状[J]. 中兽医医药杂志, 2019, 38(5):29-33 Sun Y Z, Li J Y, Wu M R, et al. Residue status of perfluoroalkyl substances in animal foods[J]. Journal of Traditional Chinese Veterinary Medicine, 2019, 38(5):29-33(in Chinese)
曹民, 邵俊娟, 高晓明, 等. 北京市昌平区市售乳制品及水果蔬菜中全氟化合物的含量及暴露评估[J]. 环境与健康杂志, 2018, 35(4):337-339 Cao M, Shao J J, Gao X M, et al. Perfluorochemicals in dairy products, vegetables and fruits in Changping district of Beijing and exposure evaluation[J]. Journal of Environment and Health, 2018, 35(4):337-339(in Chinese)
郑翌, 冷桃花, 潘煜辰, 等. 全氟化合物在食品中的污染情况及检测方法研究进展[J]. 食品工业科技, 2019, 40(10):314-319 , 333 Zheng Y, Leng T H, Pan Y C, et al. Research progress on contamination and determination methods of perfluorinated compounds in food[J]. Science and Technology of Food Industry, 2019, 40(10):314-319, 333(in Chinese)
丁林玉, 雷素珍, 曾红亮. 全氟和多氟烷基化合物的危害及在食品中的污染研究进展[J]. 食品工业科技, 2020, 41(20):336-341 , 350 Ding L Y, Lei S Z, Zeng H L. Research progress on the harm of perfluoroalkyl and polyfluoroalkyl substances and their contamination in food[J]. Science and Technology of Food Industry, 2020, 41(20):336-341, 350(in Chinese)
谢蕾, 章涛, 孙红文. 全氟烷基化合物在人体肝脏中的富集特征及其与肝损伤的关系[J]. 环境化学, 2020, 39(6):1479-1487 Xie L, Zhang T, Sun H W. Enrichment characteristics of perfluoroalkyl substances (PFASs) in human liver and its association with hepatocyte apoptosis[J]. Environmental Chemistry, 2020, 39(6):1479-1487(in Chinese)
侯沙沙, 朱会卷, 谢琳娜, 等. 人体内全氟化合物的暴露水平研究进展[J]. 环境卫生学杂志, 2020, 10(2):218-225 Hou S S, Zhu H J, Xie L N, et al. Research advances in exposure level of perfluoroalkyl and polyfluoroalkyl substances in human body[J]. Journal of Environmental Hygiene, 2020, 10(2):218-225(in Chinese)
张美, 楼巧婷, 邵倩文, 等. 全氟化合物污染现状及风险评估的研究进展[J]. 生态毒理学报, 2019, 14(3):30-53 Zhang M, Lou Q T, Shao Q W, et al. Research progress of perfluorinated compounds pollution status and risk assessment[J]. Asian Journal of Ecotoxicology, 2019, 14(3):30-53(in Chinese)
赵之梦, 张睿佳, 周枝凤, 等. 广州市某综合医院0~7岁儿童血浆中14种全氟化合物的暴露水平分析[J]. 职业与健康, 2019, 35(6):752-756 Zhao Z M, Zhang R J, Zhou Z F, et al. Analysis on plasma level of 14 perfluorinated compounds of children aged 0-7 years old in a general hospital in Guangzhou City[J]. Occupation and Health, 2019, 35(6):752-756(in Chinese)
杨帆, 施致雄. 全氟辛烷磺酸和全氟辛酸的人群暴露水平和毒性研究进展[J]. 环境与健康杂志, 2014, 31(8):730-734 Yang F, Shi Z X. Human exposure and toxicity of perfluorooctyl sulfonate and perfluorooctanoic acid:A review of recent studies[J]. Journal of Environment and Health, 2014, 31(8):730-734(in Chinese)
李磊, 周贻兵, 李海畅, 等. 牛乳中16种全氟化合物及前体物质的改进型分散固相萃取-超高效液相色谱-串联质谱快速测定法[J]. 环境与健康杂志, 2020, 37(1):76-79 Li L, Zhou Y B, Li H C, et al. Determination of sixteen perfluorochemical compounds and perfluorochemical precursors in milk by modified dispersion solid phase extraction combined with ultra high performance liquid chromatography tandem mass spectrometry[J]. Journal of Environment and Health, 2020, 37(1):76-79(in Chinese)
宋小飞, 施召才, 马伟文, 等. 液相色谱-质谱联用法测定血液中全氟化合物[J]. 分析试验室, 2020, 39(1):53-56 Song X F, Shi Z C, Ma W W, et al. Determination of perfluorinated compounds in blood by liquid chromatography mass spectrometry[J]. Chinese Journal of Analysis Laboratory, 2020, 39(1):53-56(in Chinese)
谢琳娜, 张海婧, 侯沙沙, 等. 固相萃取-超高效液相色谱-串联质谱法分析土壤中15种全氟化合物[J]. 分析化学, 2019, 47(12):1967-1972 Xie L N, Zhang H J, Hou S S, et al. Ultra performance liquid chromatography-tandem mass spectrometry coupled with solid phase extraction for determination of 15 kinds of perfluoroalkyl acid[J]. Chinese Journal of Analytical Chemistry, 2019, 47(12):1967-1972(in Chinese)
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 Y, 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 Chemistry, 2012, 31(1):113-119(in Chinese)
张妮, 胡煜钗, 夏静芬, 等. 超声萃取-柱上衍生-GC/ECD法检测污泥中的PFOS[J]. 中国给水排水, 2018, 34(10):110-114 , 118 Zhang N, Hu Y C, Xia J F, et al. Determination of PFOS in sludge by ultrasonic extraction combined with in-port derivatization-GC/ECD method[J]. China Water & Wastewater, 2018, 34(10):110-114, 118(in Chinese)
杨文宇, 赵慧, 钟琳, 等. 高效液相色谱-串联质谱法检测环境水体中18种全氟化合物[J]. 化学分析计量, 2020, 29(1):61-66 Yang W Y, Zhao H, Zhong L, et al. Determination of 18 perfluorinated alkyl substances in environmental water by high performance liquid chromatography-tandem mass spectrometry[J]. Chemical Analysis and Meterage, 2020, 29(1):61-66(in Chinese)
刘明睿, 汪伶俐, 陈亮. 超高效液相色谱串联质谱法快速测定地下水和含水层介质中16种全氟烷基酸[J]. 地学前缘, 2019, 26(4):307-314 Liu M R, Wang L L, Chen L. Quick analysis of sixteen PFAAs in groundwater and aquifer by ultra-performance liquid chromatography-triple quadrupole mass spectrometry[J]. Earth Science Frontiers, 2019, 26(4):307-314(in Chinese)
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 14 short-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(in Chinese)
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, He D C, Xu Z C, et al. Analysis of polyfluoroalkyl chemicals in water, sediments and soil by liquid chromatography-tandem mass spectrometry[J]. Environmental Monitoring in China, 2014, 30(4):134-139(in Chinese)
王晓研, 沈伟健, 王红, 等. 气相色谱-负化学源-质谱法检测水中10种全氟羧酸化合物[J]. 色谱, 2019, 37(1):32-39 Wang X Y, Shen W J, Wang H, et al. Determination of 10 perfluorinated carboxylic acid compounds in water by gas chromatography-mass spectrometry coupled with negative chemical ionization[J]. Chinese Journal of Chromatography, 2019, 37(1):32-39(in Chinese)
张俊桦, 祝玉杰, 陈来国, 等. 快速液相色谱-串联质谱法测定环境空气中的全氟化合物[J]. 生态毒理学报, 2016, 11(2):658-665 Zhang J H, Zhu Y J, Chen L G, et al. Determination of perfluorinated compounds in ambient air by rapid liquid chromatography-tandem mass spectrometry[J]. Asian Journal of Ecotoxicology, 2016, 11(2):658-665(in Chinese)
陈勇杰, 张蓓蓓, 陈国松, 等. 超高效液相色谱-串联质谱法测定污水和污泥基质中的20种全氟及多氟化合物[J]. 分析化学, 2019, 47(4):533-540 Chen Y J, Zhang B B, Chen G S, et al. Analysis of 20 kinds of perfluoroalkyl and polyfluoroalkyl substances in wastewater and sludge samples with ultra-high performance liquid chromatography-tandem mass spectrometry[J]. Chinese Journal of Analytical Chemistry, 2019, 47(4):533-540(in Chinese)
邹琴, 洪瑞申, 李康柏, 等. 废水中全氟辛酸及全氟辛磺酰基化合物的气相色谱法[J]. 广东化工, 2016, 43(9):233-234 , 236 Zou Q, Hong R S, Li K B, et al. Determination of PFOA and PFOS in wastewater using gas chromatography[J]. Guangdong Chemical Industry, 2016, 43(9):233-234, 236(in Chinese)
陈军, 杨文武, 张钧, 等. UPLC-ESI-MS/MS检测废水中11种全氟化合物[J]. 广东化工, 2015, 42(23):190-192 , 181 Chen J, Yang W W, Zhang J, et al. Determination of 11 perfluorinated compounds in waste water by UPLC-ESI-MS/MS[J]. Guangdong Chemical Industry, 2015, 42(23):190-192, 181(in Chinese)
李佩佩, 龙举, 方益, 等. 水产品中全氟化合物的分析方法和分布特征的研究进展[J]. 理化检验-化学分册, 2020, 56(6):735-744 Li P P, Long J, Fang Y, et al. Research progress on analytical methods and distribution characteristics of perfluorinated compounds in aquatic products[J]. Physical Testing and Chemical Analysis (Part B:Chemical Analysis), 2020, 56(6):735-744(in Chinese)
吴建刚, 龙强, 肖文, 等. 环境水样中全氟磺酸类和全氟羧酸类化合物分析方法研究进展[J]. 环境化学, 2018, 37(8):1851-1855 , 1857 Wu J G, Long Q, Xiao W, et al. Analytical methods of perfluorosulfonic acids (PFSAs)and perfluorocarboxylic acids (PFCAs) in environmental water samples[J]. Environmental Chemistry, 2018, 37(8):1851-1855, 1857(in Chinese)
刘殿甲, 崔明, 吴宇峰, 等. 长链全氟化合物在前处理过程中的吸附情况研究[J]. 分析试验室, 2020, 39(5):600-604 Liu D J, Cui M, Wu Y F, et al. Study on adsorption of long chain perfluorinated compounds during sample pretreatment[J]. Chinese Journal of Analysis Laboratory, 2020, 39(5):600-604(in Chinese)
贺思思, 史亚利, 蔡亚岐, 等. 全氟/多氟化合物分析方法的研究进展[J]. 色谱, 2020, 38(3):287-296 He S S, Shi Y L, Cai Y Q, et al. Research progress on the analytical method of perfluoroalkyl and polyfluoroalkyl substances[J]. Chinese Journal of Chromatography, 2020, 38(3):287-296(in Chinese)
贺锦灿, 张诗韵, 苏榆媛, 等. 典型全氟有机酸类化合物的样品前处理与分析方法研究进展[J]. 色谱, 2020, 38(1):86-94 He J C, Zhang S Y, Su Y Y, et al. Progress on the sample techniques and analytical methods for typical perfluorinated organic acids[J]. Chinese Journal of Chromatography, 2020, 38(1):86-94(in Chinese)
陈鑫, 刘杰, 曾晓岚, 等. 全氟辛酸污染及检测方法的研究进展[J]. 环境科学与技术, 2019, 42(5):125-134 Chen X, Liu J, Zeng X L, et al. Review on the pollution status and detection methods of perfluorooctanoic acid[J]. Environmental Science & Technology, 2019, 42(5):125-134(in Chinese)
United States Environmental Protection Agency (US EPA). Method 537.1 determination of selected per- and polyflourinated alkyl substances in drinking water by solid phase extraction and liquid chromatography/tandem mass spectrometry (LC/MS/MS)[S]. Washington DC:Office of Water, Office of Science and Technology, 2018 United States Environmental Protection Agency (US EPA). Method 8327 per-and polyfluoroalkyl substances (PFAS) using external standard calibration and multiple reaction monitoring (MRM) liquid chromatography/tandem mass spectrometry (LC/MS/MS)[S]. Washington DC:Office of Water, Office of Science and Technology, 2019 盛龙生, 苏焕华, 郭丹滨. 色谱质谱联用技术[M]. 北京:化学工业出版社, 2006:103-104 中华人民共和国生态环境部. HJ91.1-2019污水监测技术规范[S]. 北京:中国环境出版集团, 2019 Sun H W, Li F S, Zhang T, et al. Perfluorinated compounds in surface waters and WWTPs in Shenyang, China:Mass flows and source analysis[J]. Water Research, 2011, 45(15):4483-4490 Sun H W, Zhang X Z, Wang L, et al. Perfluoroalkyl compounds in municipal WWTPs in Tianjin, China-Concentrations, distribution and mass flow[J]. Environmental Science and Pollution Research, 2012, 19(5):1405-1415 Ahrens L, Felizeter S, Sturm R, et al. Polyfluorinated compounds in waste water treatment plant effluents and surface waters along the River Elbe, Germany[J]. Marine Pollution Bulletin, 2009, 58(9):1326-1333 Campo J, Masiá A, Picó Y, et al. Distribution and fate of perfluoroalkyl substances in Mediterranean Spanish sewage treatment plants[J]. Science of the Total Environment, 2014, 472:912-922 Shivakoti B R, Tanaka S, Fujii S, et al. Occurrences and behavior of perfluorinated compounds (PFCs) in several wastewater treatment plants (WWTPs) in Japan and Thailand[J]. Journal of Environmental Monitoring, 2010, 12(6):1255-1264 -
点击查看大图
计量
- 文章访问数: 2614
- HTML全文浏览数: 2614
- PDF下载数: 76
- 施引文献: 0
下载:
