超高效液相色谱-高分辨质谱法同时测定鱼肉中16种全氟烷基化合物

引用本文: 涂祥婷, 杨鸿波, 郭峰, 曾士宜, 滕春丽, 孙晓红, 何锦林, 林绍霞. 超高效液相色谱-高分辨质谱法同时测定鱼肉中16种全氟烷基化合物[J]. 分析化学, 2021, 49(4): 528-537. doi: 10.19756/j.issn.0253-3820.211007 shu

Citation: TU Xiang-Ting, YANG Hong-Bo, GUO Feng, ZENG Shi-Yi, TENG Chun-Li, SUN Xiao-Hong, HE Jin-Lin, LIN Shao-Xia. Simultaneous Determination of 16 Kinds of Perfluoroalkyl Substances in Fish Muscle by Ultra High Performance Liquid Chromatography-High Resolution Mass Spectrometry[J]. Chinese Journal of Analytical Chemistry, 2021, 49(4): 528-537. doi: 10.19756/j.issn.0253-3820.211007 shu

超高效液相色谱-高分辨质谱法同时测定鱼肉中16种全氟烷基化合物

涂祥婷 ^1,2,3, ,
杨鸿波 ^{1,3,
,} ,
郭峰 ^{2,
,} ,
曾士宜 ^3, ,
滕春丽 ^1,3, ,
孙晓红 ^1, ,
何锦林 ^3, ,
林绍霞 ^3,

1.
贵州医科大学公共卫生学院, 环境污染与疾病监控教育部重点实验室, 贵阳 550025;
2.
国家地质实验测试中心, 自然资源部生态地球化学重点实验室, 北京 100037;
3.
贵州省分析测试研究院, 贵阳 550016

通讯作者: 杨鸿波,E-mail:hbyang@gzata.cn; 郭峰,E-mail:fengguo@cags.ac.cn

基金项目:
国家自然科学基金项目（Nos.21966011，21976044）、中央引导地方科技发展专项资金项目（No.黔科中引地[2016]4001）和中央级公益性科研院所基本科研业务费项目（No.CSJ201906）资助。

摘要: 建立了快速滤过型净化（Multi-plug filtration cleanup，m-PFC）-超高效液相色谱-四极杆-静电场离子轨道阱高分辨质谱法同时测定鱼肉中16种全氟烷基化合物（Perfluorinated alkylated substances，PFASs）。样品经1%甲酸-乙腈溶液超声提取，通过式m-PFC固相萃取柱净化，氮吹浓缩至1 mL后，以AcquityWaters BEH C₁₈色谱柱（50 mm×2.1 mm，1.7 μm）分离，甲醇-5 mmol/L乙酸铵溶液进行梯度洗脱。质谱采用Full MS/dd-MS²扫描模式，正离子和负离子切换扫描，采用内标法进行定量分析。在最佳的分析条件下，16种目标物在13 min内均可实现良好分离，各物质的精确质量数偏差均小于2.83×10^-6，在0.10-20.0 μg/L浓度范围内，各化合物线性关系良好，相关系数（R²）均大于0.990，方法的检出限为0.015-0.05 μg/kg。在0.50、2.0和5.0 μg/kg的基质加标水平下，平均回收率为70.7%-110.1%，相对标准偏差（Relative standard deviations，RSDs）为0.5%-12.8%。将本方法应用于25个野生鱼样品的快速分析，共检出10种PFASs，其中全氟辛酸（Perfluorooctane sulfonate，PFOS）为主要污染物。本方法操作简单、快速、准确度高、灵敏度高，适用于鱼肉中16种PFASs的快速检测。

关键词:

English

Simultaneous Determination of 16 Kinds of Perfluoroalkyl Substances in Fish Muscle by Ultra High Performance Liquid Chromatography-High Resolution Mass Spectrometry

1.
The Key Laboratory of Environmental Pollution Monitoring and Disease Control, Ministry of Education, School of Public Health, Guizhou Medical University, Guiyang 550025, China;
2.
Key Laboratory of Eco-Geochemistry, Ministry of Natural Resources, National Research Center for Geoanalysis, Beijing 100037, China;
3.
Guizhou Academy of Testing and Analysis, Guiyang 550016, China

Corresponding author: YANG Hong-Bo, ; GUO Feng,

Received Date: 05 January 2021
Revised Date: 02 March 2021
Fund Project:
Supported by the National Natural Science Foundation of China (Nos.21966011, 21976044), the Central Government leading Local Science and Technology Development (No.Qian Ke-Zhong Yin Dit [2016]4001), and the Central Undertakings Basic Research Expenses Special Funds (No.CSJ 201906).

Abstract: A method for determination of 16 kinds of perfluoroalkyl substances in fish muscle by multi-plug filtration cleanup (m-PFC) combined with ulrahigh performance liquid chromatography-Q-extractive orbitrap high resolution mass spectrometry (UHPLC-Q-Orbitrap HRMS) was established. The samples were ultrasonically extracted by 1% formic acid-acetonitrile, purified by solid phase extraction using m-PFC column and concentrated to 1 mL under nitrogen. The analytes were separated on an Acquity Waters BEH C₁₈ (50 mm×2.1 mm, 1.7 μm) column, and gradient eluted with 5 mmol/L ammonium acetate and methanol. The MS acquisition mode was Full MS/dd-MS² in both negative and positive ionization mode, and the internal standard method was used for quantification. Under the best analytical conditions, a total of 16 target compounds were well separated within 13 min, and the accurate mass deviation of each substance was less than 2.83×10^-6. A good linearity was obtained in the concentration ranges of 0.10-20.0 μg/L with correlation coefficients of greater than 0.990. The MDLs ranged from 0.015 μg/kg to 0.05 μg/kg. The average recoveries of 16 kinds of PFASs spiked at 0.50, 2.0 and 5.0 μg/kg were 70.7%-110.1% and the relative standard deviations (RSDs) were 0.5%-12.8%. The established method was successfully applied to the rapid detection of 25 wild fish samples. Ten PFASs were detected, in which PFOS were the predominant pollutant. The method was simple, rapid, accurate and sensitive, and suitable for the rapid detection of 16 kinds of PFASs in fish muscle.

Key words:

Q-Exactive orbitrap plus high resolution mass spectrometry
/ Multi-plug filtration cleanup
/ Fish muscle
/ Perfluorinated alkylated substances

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

超高效液相色谱-高分辨质谱法同时测定鱼肉中16种全氟烷基化合物

通讯作者: 杨鸿波,E-mail:hbyang@gzata.cn; 郭峰,E-mail:fengguo@cags.ac.cn

English

Simultaneous Determination of 16 Kinds of Perfluoroalkyl Substances in Fish Muscle by Ultra High Performance Liquid Chromatography-High Resolution Mass Spectrometry

Corresponding author: YANG Hong-Bo, ; GUO Feng,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

超高效液相色谱-高分辨质谱法同时测定 鱼肉中16种全氟烷基化合物

通讯作者: 杨鸿波,E-mail:hbyang@gzata.cn; 郭峰,E-mail:fengguo@cags.ac.cn

English

Simultaneous Determination of 16 Kinds of Perfluoroalkyl Substances in Fish Muscle by Ultra High Performance Liquid Chromatography-High Resolution Mass Spectrometry

Corresponding author: YANG Hong-Bo, ; GUO Feng,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

超高效液相色谱-高分辨质谱法同时测定鱼肉中16种全氟烷基化合物

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs