液相色谱保留时间指标在基于 HRMS 的可疑物和非目标物筛查中的开发与应用,Analytical Chemistry

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液相色谱保留时间指标在基于 HRMS 的可疑物和非目标物筛查中的开发与应用
Analytical Chemistry ( IF 7.4 ) Pub Date : 2021-08-12 , DOI: 10.1021/acs.analchem.1c02348
Reza Aalizadeh ₁ , Nikiforos A Alygizakis _{1,

2} , Emma L Schymanski _{3,

4} , Martin Krauss ₅ , Tobias Schulze ₅ , María Ibáñez ₆ , Andrew D McEachran ₇ , Alex Chao ₇ , Antony J Williams ₇ , Pablo Gago-Ferrero _{8,

9} , Adrian Covaci ₁₀ , Christoph Moschet ₁₁ , Thomas M Young ₁₁ , Juliane Hollender _{4,

12} , Jaroslav Slobodnik ₂ , Nikolaos S Thomaidis ₁

Affiliation

Laboratory of Analytical Chemistry, Department of Chemistry, National and Kapodistrian University of Athens, Panepistimiopolis Zografou, 157 71 Athens, Greece.
Environmental Institute, Okružná 784/42, 97241 Koš, Slovak Republic.
Luxembourg Centre for Systems Biomedicine (LCSB), University of Luxembourg, 6 Avenue du Swing, L-4367 Belvaux, Luxembourg.
Eawag: Swiss Federal Institute for Aquatic Science and Technology, Überlandstrasse 133, 8600 Dübendorf, Switzerland.
Department Effect-Directed Analysis, Helmholtz-Centre for Environmental Research-UFZ, Leipzig, Germany.
Research Institute for Pesticides and Water, University Jaume I, Castellón 12071, Spain.
Center for Computational Toxicology and Exposure, Office of Research and Development, U.S. Environmental Protection Agency, Mail Drop, D143-02, 109 T.W. Alexander Dr., Research Triangle Park, North Carolina 27711, United States.
Institute of Environmental Assessment and Water Research (IDAEA) Severo Ochoa Excellence Center, Spanish Council for Scientific Research (CSIC), Jordi Girona 18-26, E-08034 Barcelona, Spain.
Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), P. O. Box 7050, SE-750 07 Uppsala, Sweden.
Toxicological Center, University of Antwerp, 2610 Wilrijk, Belgium.
Department of Civil and Environmental Engineering, University of California, Davis, California 95616, United States.
Institute of Biogeochemistry and Pollutant Dynamics, IBP, ETH Zurich, 8092 Zurich, Switzerland.

越来越需要可比较和统一的保留时间 ( t _R) 在不同实验室之间的液相色谱 (LC) 中，为基于高分辨率质谱 (HRMS) 的可疑和非目标筛查调查中的化合物鉴定提供补充证据。在本研究中，基于洗脱模式的校准，提出了一种经过严格测试、灵活且不太依赖系统的 LC 统一保留时间指数 (RTI) 方法。根据与 2123 种化合物的保留时间和化学相似性指数的最大重叠，为 ESI+ 和 ESI-中的每一个选择了两组 18 种校准物。由此产生的校准集，RTI 设置在 1 到 1000 之间，经过严格评估，由 NORMAN 网络协调，被提议为最合适的 RTI 系统。建议的 RTI 系统的验证是在不同仪器和 LC 条件下在外部完成的。RTI 还可用于检查 LC 条件的重现性和质量。基于开发的 RTI 系统建立了两个基于定量结构保留关系 (QSRR) 的模型，这些模型有助于去除假阳性注释。QSRR 模型的适用性域允许以更高的置信度完成识别过程，同时指示应谨慎处理结果的那些物质。提议的 RTI 系统用于提高对可疑和非目标筛查的信心，并增加实验室之间的可比性，如两个例子所示。所有与 RTI 相关的计算都可以在 http://rti.chem.uoa.gr/ 上在线进行。

"点击查看英文标题和摘要"

Development and Application of Liquid Chromatographic Retention Time Indices in HRMS-Based Suspect and Nontarget Screening

There is an increasing need for comparable and harmonized retention times (t_R) in liquid chromatography (LC) among different laboratories, to provide supplementary evidence for the identity of compounds in high-resolution mass spectrometry (HRMS)-based suspect and nontarget screening investigations. In this study, a rigorously tested, flexible, and less system-dependent unified retention time index (RTI) approach for LC is presented, based on the calibration of the elution pattern. Two sets of 18 calibrants were selected for each of ESI+ and ESI-based on the maximum overlap with the retention times and chemical similarity indices from a total set of 2123 compounds. The resulting calibration set, with RTI set to range between 1 and 1000, was proposed as the most appropriate RTI system after rigorous evaluation, coordinated by the NORMAN network. The validation of the proposed RTI system was done externally on different instrumentation and LC conditions. The RTI can also be used to check the reproducibility and quality of LC conditions. Two quantitative structure–retention relationship (QSRR)-based models were built based on the developed RTI systems, which assist in the removal of false-positive annotations. The applicability domains of the QSRR models allowed completing the identification process with higher confidence for substances within the domain, while indicating those substances for which results should be treated with caution. The proposed RTI system was used to improve confidence in suspect and nontarget screening and increase the comparability between laboratories as demonstrated for two examples. All RTI-related calculations can be performed online at http://rti.chem.uoa.gr/.

更新日期：2021-08-24

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