HDPairFinder:A data processing platform for hydrogen/deuterium isotopic labeling-based nontargeted analysis of trace-level amino-containing chemicals in environmental water

查看全文 作　　者：Tingting [1]Zhao;Kristin [2]Carroll;Caley [2]B.Craven;Nicholas [2]J.P.Wawryk;Shipei [1]Xing;Jian [1]Guo;Xing-Fang [2]Li;Tao [1]Huan 机构地区：[1]Department of Chemistry,Faculty of Science,University of British Columbia,Vancouver Campus,2036 Main Mall,Vancouver,British Columbia,V6T 1Z1,Canada;[2]Division of Analytical and Environmental Toxicology,Department of Laboratory Medicine and Pathology,Faculty of Medicine and Dentistry,University of Alberta,Edmonton,Alberta T6G 2G3,Canada 出　　处：《Journal of Environmental Sciences》索引2024年第2期,共11页 基　　金：supported by grants from the Natural Sciences and Engineering Research Council of Canada,Alberta Innovates;the Canada Research Chairs Program。 摘　　要：The combination of hydrogen/deuterium(H/D)formaldehyde-based isotopic methyl labeling with solid-phase extraction and high-performance liquid chromatography–high resolution mass spectrometry(HPLC-HRMS)is a powerful analytical solution for nontargeted analysis of trace-level amino-containing chemicals in water samples.Given the huge amount of chemical information generated in HPLC-HRMS analysis,identifying all possible H/Dlabeled amino chemicals presents a significant challenge in data processing.To address this,we designed a streamlined data processing pipeline that can automatically extract H/D-labeled amino chemicals from the raw HPLC-HRMS data with high accuracy and efficiency.First,we developed a cross-correlation algorithm to correct the retention time shift resulting from deuterium isotopic effects,which enables reliable pairing of H-and D-labeled peaks.Second,we implemented several bioinformatic solutions to remove false chemical features generated by in-source fragmentation,salt adduction,and natural13C isotopes.Third,we used a data mining strategy to construct the AMINES library that consists of over 38,000 structure-disjointed primary and secondary amines to facilitate putative compound annotation.Finally,we integrated these modules into a freely available R program,HDPairFinder.R.The rationale of each module was justified and its performance tested using experimental H/D-labeled chemical standards and authentic water samples.We further demonstrated the application of HDPairFinder to effectively extract N-containing contaminants,thus enabling the monitoring of changes of primary and secondary N-compounds in authentic water samples.HDPairFinder is a reliable bioinformatic tool for rapid processing of H/D isotopic methyl labeling-based nontargeted analysis of water samples,and will facilitate a better understanding of N-containing chemical compounds in water. 关 键 词：Isotope labeling Nontargeted analysis Reactive N-compounds HPLC-HRMS Source water