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非抑制型离子色谱串联质谱法同时测定饮用水中卤乙酸和卤氧化物

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程士, 吴亚萍, 左延婷, 钱玉亭, 李爱民, 霍宗利, 李文涛. 非抑制型离子色谱串联质谱法同时测定饮用水中卤乙酸和卤氧化物[J]. 环境化学, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
引用本文: 程士, 吴亚萍, 左延婷, 钱玉亭, 李爱民, 霍宗利, 李文涛. 非抑制型离子色谱串联质谱法同时测定饮用水中卤乙酸和卤氧化物[J]. 环境化学, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
shu
CHENG Shi, WU Yaping, ZUO Yanting, QIAN Yuting, LI Aimin, HUO Zongli, LI Wentao. Simultaneous determination of haloacetic acids and oxyhalides in drinking water by non-suppressed ion chromatography-tandem mass spectrometry[J]. Environmental Chemistry, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
Citation: CHENG Shi, WU Yaping, ZUO Yanting, QIAN Yuting, LI Aimin, HUO Zongli, LI Wentao. Simultaneous determination of haloacetic acids and oxyhalides in drinking water by non-suppressed ion chromatography-tandem mass spectrometry[J]. Environmental Chemistry, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
shu

非抑制型离子色谱串联质谱法同时测定饮用水中卤乙酸和卤氧化物

  • 1. 南京大学环境学院, 污染控制与资源化研究国家重点实验室, 南京, 210023;

  • 2. 江阴市环境监测站, 江阴, 214400;

  • 3. 江苏省疾病预防控制中心, 南京, 210009

    • 通讯作者: 霍宗利, E-mail: huozong123@163.com ;  李文涛, E-mail: liwentao@nju.edu.cn
  • 基金项目:

    国家自然科学基金（51708279），国家重点研发计划（2016YFE0112300），江苏省基础研究计划（BK20170642）和生活饮用水中消毒副产物标准检验方法研制项目（中疾控环协合同水发[2019]1-3号）资助.

Simultaneous determination of haloacetic acids and oxyhalides in drinking water by non-suppressed ion chromatography-tandem mass spectrometry

  • 1. State Key Laboratory of Pollution Control and Resources Reuse, School of the Environment, Nanjing University, Nanjing, 210023, China;

  • 2. Jiangyin Environmental Monitoring Station, Jangyin, 214400, China;

  • 3. Jiangsu Provincial Center for Disease Control and Prevention, Nanjing, 210009, China

    • Corresponding authors: HUO Zongli, huozong123@163.com ;  LI Wentao, liwentao@nju.edu.cn
  • Fund Project: Supported by the National Natural Science Foundation of China(51708279), National Key R&D Program (2016YFE0112300), Basic Research Program of Jiangsu Province (BK20170642) and Research and Development Project of Standard Examination Method for Disinfection by-Products in Drinking Water (Contract No.1-3[2019] Issued by China Association for Disease Control and Environmental Protection).

摘要

  • 摘要: 本文建立了一种基于非离子抑制型离子色谱-电喷雾离子化-串联质谱（IC-ESI-MS/MS）的卤乙酸和卤氧化物分析方法，解决了当前卤乙酸检测预处理过程复杂和卤氧化物检测灵敏度低的问题，本方法中仅需的样品前处理为0.45 μm滤膜过滤.样品采用Dionex IonPac AS16色谱柱进行分离，使用甲胺水溶液和乙腈作为混合流动相.采用电喷雾负离子（ESI-）模式，多反应监测模式（MRM）进行质谱分析.本文系统研究了甲胺水溶液的浓度及比例对分析物保留时间和响应值的影响，确定最优流动相条件为0.7 mol·L-1甲胺水溶液/乙腈，体积比30/70，等度洗脱.在此条件下，9种卤乙酸和3种卤氧化物在0.5-100 μg·L-1范围内均具有很好的线性关系（r>0.995），检出限为0.052-0.270 μg·L-1，检测下限为0.208-1.080 μg·L-1；在自来水中加标回收率为74.9%-114.9%，相对标准偏差为1.2%-8.7%.运用本方法对模拟加氯消毒水样及无锡市的自来水进行检测，两次测量结果偏差小，二氯乙酸和三氯乙酸检出浓度最高.本方法灵敏快速、操作简便，为国家标准《生活饮用水标准检验方法》（GB/T5750）中二氯乙酸、三氯乙酸、氯酸盐和溴酸盐等指标的检测方法修订提供了技术支撑.
    Abstract: An determination method of haloacetic acids (HAAs) and oxyhalides using non-suppressed ion chromatography electrospray ionization tandem mass spectrometry (IC-ESI-MS/MS) was established to solve the problems of complex pretreatment for HAAs detection and the low sensitivity for oxyhalides detection. In this method, the only pretreatment was the process of 0.45 μm membrane filtration. The samples were separated by Dionex IonPac AS16 column, and aqueous methylamine solution and acetonitrile were used as the mixed mobile phases. Negative electrospray ionization (ESI-) mode and multiple reaction monitoring mode (MRM) were used for mass spectrometry analysis. The effects of concentration and proportion of aqueous methylamine solution on retention time and response value of the analytes were studied, and the optimal mobile phase condition was determined to be 0.7 mol·L-1 aqueous methylamine solution/acetonitrile, with a volume ratio of 30/70 and elution in equal degree. Under the optimal condition, all of the 12 analytes had good linear relationships(r>0.995)in the range of 0.5-100 μg·L-1, with the detection limits of 0.052-0.270 μg·L-1, the minimum quantitative detection limits of 0.208-1.080 μg·L-1. The recoveries of the spiked 12 analytes in tap water were 74.9%-114.9% with relative standard deviations ranging from 1.2% to 9.0%. This method was applied to analyze the simulated chlorinated water and tap water from Wuxi. The deviation of the duplicate analyses was small, and the concentrations of dichloroacetic acid and trichloroacetic acid were the highest. This method is sensitive, rapid and easy to operate, which provides technical support for the revision of the detection methods of dichloroacetic acid, trichloroacetic acid, chlorate and bromate in the "Standard Examination Method for Drinking Water" (GB/T5750).
  • [1] KRASNER S W, WEINBERG H S, RICHARDSON S D, et al. Occurrence of a new generation of disinfection byproducts[J]. Environmental Science & Technology, 2006, 40(23):7175-7185.
    [2] PALS J A, ANG J K, WAGNER E D, et al. Biological mechanism for the toxicity of haloacetic acid drinking water disinfection by-products[J]. Environmental Science & Technology, 2011, 45(13):5791-5797.
    [3] ESCOBARHOYOS L F, HOYOSGIRALD L S, LONDONOVELASCO E, et al. Genotoxic and clastogenic effects of monohaloacetic acid drinking water disinfection by-products in primary human lymphocytes[J]. Water Research, 2013, 47(10):3282-3290.
    [4] XU X, GAO B Y, JIN B, et al. Study of microbial perchlorate reduction:Considering of multiple pH, electron cceptors and donors[J]. Journal of Hazardous Materials, 2015, 285:228-235.
    [5] 尹江伟, 刘祖强, 李红华, 等. 离子色谱法测定饮用水中3种加氯消毒副产物[J]. 中国热带医学, 2004, 4(3):458-459.

    YIN J W, LIU Z Q, LI H H, et al. Determination of three by-products by using ion chromatography after adding chloride disinfectant in the drinking water[J]. China Tropical Medicine, 2004, 4(3):458-459(in Chinese).

    [6] 陈际, 周永芳, 杜双双, 等. 超高效液相色谱-串联质谱法检测饮用水中二氯乙酸和三氯乙酸[J]. 净水技术, 2018, 37(4):66-70.

    CHEN J, ZHOU Y F, DU S S, et al. Determination of dichloroacetic acid and trichloroacetic acid in drinking water by ultra performance liquid chromatography-tandem mass spectrometry(UPLC-MS/MS)[J]. Water Purification Technology, 2018, 37(4):66-70(in Chinese).

    [7] 李宗来, 何琴. 超高效液相色谱串联质谱法检测饮用水中卤乙酸[J]. 环境化学, 2011, 30(2):574-576.

    LI Z L, HE Q. Determination of haloacetic acid in drinking water by ultra high performance liquid chromatography tandem mass spectrometry[J]. Environmental Chemistry, 2011, 30(2):574-576(in Chinese).

    [8] LIU Y, MOU S, CHEN D. Determination of trace-level haloacetic acids in drinking water by ion chromatography-inductively coupled plasma mass spectrometry[J]. Journal of Chromatography A, 2004, 1039(1/2):89-95.
    [9] 苏宇亮, 冯兆敏, 胡克武, 等. 离子色谱法测定水中的卤代乙酸和卤素含氧酸[J]. 中国给水排水, 2006,22(12):86-88.

    SU Y L, FENG Z M, HU K W, et al. Determination of haloacetic acids and haloid oxyacids by ion chromatographic method[J]. China Water & Wastewater, 2006,22(12):86-88(in Chinese).

    [10] BRUZZONINITI M C, DE CARLO R M, HORVATH K, et al. High performance ion chromatography of haloacetic acids on macrocyclic cryptand anion exchanger[J]. Journal of Chromatography A, 2008, 1187(1/2):188-196.
    [11] 钟新林. 离子色谱法测定饮用水中亚氯酸盐、氯酸盐、溴酸盐、二氯乙酸及三氯乙酸[J]. 环境化学, 2013, 32(7):1422-1423.

    ZHONG X L. Determination of chlorite, chlorate, bromate, dichloroacetic acid and trichloroacetic acid in drinking water by Ion Chromatography[J]. Environmental Chemistry, 2013, 32(7):1422-1423(in Chinese).

    [12] MENG L P, WU S M, MA F J, et al. Trace determination of nine haloacetic acids in drinking water by liquid chromatography-electrospray tandem mass spectrometry[J]. Journal of Chromatography A, 2010, 1217(29):4873-4876.
    [13] 雷颖, 八十岛诚, 王凌云, 等. 液相色谱-串联质谱法同时检测自来水中9种卤乙酸[J]. 中国给水排水, 2013, 29(20):124-129.

    LEI Y, YASOJIMA M, WANG L Y, et al. Determination of nine haloacetic acids in tap water by liquid chromatography-tandem mass spectrometry[J]. China Water & Wastewater, 2013, 29(20):124-129(in Chinese).

    [14] 李建中, 陈伟, 薄涛,等. 生活饮用水中消毒副产物卤乙酸的UHPLC-MS/MS分析[J]. 环境化学, 2012, 31(5):757-759.

    LI J Z, CHEN W, BO T, et al. Analysis of haloacetic acid in drinking water by UHPLC-MS/MS[J]. Environmental Chemistry, 2012, 31(5):757-759(in Chinese).

    [15] DUAN J, LI W, SI J, et al. Rapid determination of nine haloacetic acids in water using ultra-performance liquid chromatography-tandem mass spectrometry in multiple reactions monitoring mode[J]. Analytical Methods, 2011, 3(7):1667-1673.
    [16] 贾娜, 张辰凌, 刘冰冰, 等. 离子色谱法快速测定饮用水中4种卤氧化合物[J]. 理化检验(化学分册), 2019, 55(11

    ):1337-1340. JIA N, ZHANG C L, LIU B B, et al. Rapid determination of four oxyhalides in drinking water by ion chromatography[J]. Physical Testing and Chemical Analysis(Part B:Chemical Analysis), 2019, 55(11):1337-1340(in Chinese).

    [17] TEH H B, LI S F Y. Simultaneous determination of bromate, chlorite and haloacetic acids by two-dimensional matrix elimination ion chromatography with coupled conventional and capillary columns[J]. Journal of Chromatography A, 2015, 1383:112-120.
    [18] USEPA, Method 557, Version 1.0. Determination of Haloacetic Acids, Bromate, and Dalapon in Drinking Water by Ion Chromatography Electrospray Ionization Tandem Mass Spectrometry[S]. 2009.
    [19] LI W T, CAO M J, YOUNG T, et al. Application of UV absorbance and fluorescence indicators to assess the formation of biodegradable dissolved organic carbon and bromate during ozonation[J]. Water Research, 2017, 111:154-162.

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  • 收稿日期:  2020-05-18
程士, 吴亚萍, 左延婷, 钱玉亭, 李爱民, 霍宗利, 李文涛. 非抑制型离子色谱串联质谱法同时测定饮用水中卤乙酸和卤氧化物[J]. 环境化学, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
引用本文: 程士, 吴亚萍, 左延婷, 钱玉亭, 李爱民, 霍宗利, 李文涛. 非抑制型离子色谱串联质谱法同时测定饮用水中卤乙酸和卤氧化物[J]. 环境化学, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
shu
CHENG Shi, WU Yaping, ZUO Yanting, QIAN Yuting, LI Aimin, HUO Zongli, LI Wentao. Simultaneous determination of haloacetic acids and oxyhalides in drinking water by non-suppressed ion chromatography-tandem mass spectrometry[J]. Environmental Chemistry, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
Citation: CHENG Shi, WU Yaping, ZUO Yanting, QIAN Yuting, LI Aimin, HUO Zongli, LI Wentao. Simultaneous determination of haloacetic acids and oxyhalides in drinking water by non-suppressed ion chromatography-tandem mass spectrometry[J]. Environmental Chemistry, 2020, (11): 3064-3071. doi: 10.7524/j.issn.0254-6108.2020051804
shu

非抑制型离子色谱串联质谱法同时测定饮用水中卤乙酸和卤氧化物

    通讯作者: 霍宗利, E-mail: huozong123@163.com ;  李文涛, E-mail: liwentao@nju.edu.cn
  • 1. 南京大学环境学院, 污染控制与资源化研究国家重点实验室, 南京, 210023;
  • 2. 江阴市环境监测站, 江阴, 214400;
  • 3. 江苏省疾病预防控制中心, 南京, 210009
  • 收稿日期:  2020-05-18
基金项目:

国家自然科学基金（51708279），国家重点研发计划（2016YFE0112300），江苏省基础研究计划（BK20170642）和生活饮用水中消毒副产物标准检验方法研制项目（中疾控环协合同水发[2019]1-3号）资助.

摘要: 本文建立了一种基于非离子抑制型离子色谱-电喷雾离子化-串联质谱（IC-ESI-MS/MS）的卤乙酸和卤氧化物分析方法，解决了当前卤乙酸检测预处理过程复杂和卤氧化物检测灵敏度低的问题，本方法中仅需的样品前处理为0.45 μm滤膜过滤.样品采用Dionex IonPac AS16色谱柱进行分离，使用甲胺水溶液和乙腈作为混合流动相.采用电喷雾负离子（ESI-）模式，多反应监测模式（MRM）进行质谱分析.本文系统研究了甲胺水溶液的浓度及比例对分析物保留时间和响应值的影响，确定最优流动相条件为0.7 mol·L-1甲胺水溶液/乙腈，体积比30/70，等度洗脱.在此条件下，9种卤乙酸和3种卤氧化物在0.5-100 μg·L-1范围内均具有很好的线性关系（r>0.995），检出限为0.052-0.270 μg·L-1，检测下限为0.208-1.080 μg·L-1；在自来水中加标回收率为74.9%-114.9%，相对标准偏差为1.2%-8.7%.运用本方法对模拟加氯消毒水样及无锡市的自来水进行检测，两次测量结果偏差小，二氯乙酸和三氯乙酸检出浓度最高.本方法灵敏快速、操作简便，为国家标准《生活饮用水标准检验方法》（GB/T5750）中二氯乙酸、三氯乙酸、氯酸盐和溴酸盐等指标的检测方法修订提供了技术支撑.

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