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 a...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.展开更多
Cannabis is increasingly used for both medicinal and recreational purposes with an estimate of over 180 million users annually.Canada has recently legalized cannabis use in October 2018,joining several states,in the U...Cannabis is increasingly used for both medicinal and recreational purposes with an estimate of over 180 million users annually.Canada has recently legalized cannabis use in October 2018,joining several states,in the United States of America (e.g.,Colorado,California,and Oregon) and a few other countries.A variety of cannabis products including dry flowers,edibles,and oil products are widely consumed.With high demand for cannabis products worldwide,the quality of cannabis and its related products has become a major concern for consumer safety.Various guidelines have been set by different countries to ensure the quality,safety,and efficacy of cannabis products.In general,these guidelines require control of contaminants including pesticides,toxic elements,mycotoxins,and pathogens,as well as residual solvents in regard to cannabis oil.Accordingly,appropriate analytical methods are required to determine these contaminants in cannabis products for quality control.In this review,we focus on the current analytical challenges and method development for detection of pesticides and toxic elements in cannabis to meet various guidelines.展开更多
Disinfection byproducts(DBPs)represent a ubiquitous source of chemical exposure in disinfected water.While over 700 DBPs have been identified,the drivers of toxicity remain poorly understood.Additionally,ever evolving...Disinfection byproducts(DBPs)represent a ubiquitous source of chemical exposure in disinfected water.While over 700 DBPs have been identified,the drivers of toxicity remain poorly understood.Additionally,ever evolving water treatment practices have led to a continually growing list of DBPs.Advancement of analytical technologies have enabled the identification of new classes of DBPs and the quantification of these chemically diverse sets of DBPs.Here we summarize advances in new workflows for DBP analysis,including sample preparation,chromatographic separation with mass spectrometry(MS)detection,and data processing.To aid in the selection of techniques for future studies,we discuss necessary considerations for each step in the strategy.This review focuses on how each step of a workflow can be optimized to capture diverse classes of DBPs within a single method.Additionally,we highlight new MS-based approaches that can be powerful for identifying novel DBPs of toxicological relevance.We discuss current challenges and provide perspectives on future research directions with respect to studying new DBPs of toxicological relevance.As analytical technologies continue to advance,new strategies will be increasingly used to analyze complex DBPs produced in different treatment processes with the aim to identify potential drivers of toxicity.展开更多
基金supported by grants from the Natural Sciences and Engineering Research Council of Canada,Alberta Innovatesthe Canada Research Chairs Program。
文摘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.
基金the Natural Sciences and Engineering Research Council of Canada(NSERC)for their ongoing funding support of the Li group through various research grants
文摘Cannabis is increasingly used for both medicinal and recreational purposes with an estimate of over 180 million users annually.Canada has recently legalized cannabis use in October 2018,joining several states,in the United States of America (e.g.,Colorado,California,and Oregon) and a few other countries.A variety of cannabis products including dry flowers,edibles,and oil products are widely consumed.With high demand for cannabis products worldwide,the quality of cannabis and its related products has become a major concern for consumer safety.Various guidelines have been set by different countries to ensure the quality,safety,and efficacy of cannabis products.In general,these guidelines require control of contaminants including pesticides,toxic elements,mycotoxins,and pathogens,as well as residual solvents in regard to cannabis oil.Accordingly,appropriate analytical methods are required to determine these contaminants in cannabis products for quality control.In this review,we focus on the current analytical challenges and method development for detection of pesticides and toxic elements in cannabis to meet various guidelines.
文摘Disinfection byproducts(DBPs)represent a ubiquitous source of chemical exposure in disinfected water.While over 700 DBPs have been identified,the drivers of toxicity remain poorly understood.Additionally,ever evolving water treatment practices have led to a continually growing list of DBPs.Advancement of analytical technologies have enabled the identification of new classes of DBPs and the quantification of these chemically diverse sets of DBPs.Here we summarize advances in new workflows for DBP analysis,including sample preparation,chromatographic separation with mass spectrometry(MS)detection,and data processing.To aid in the selection of techniques for future studies,we discuss necessary considerations for each step in the strategy.This review focuses on how each step of a workflow can be optimized to capture diverse classes of DBPs within a single method.Additionally,we highlight new MS-based approaches that can be powerful for identifying novel DBPs of toxicological relevance.We discuss current challenges and provide perspectives on future research directions with respect to studying new DBPs of toxicological relevance.As analytical technologies continue to advance,new strategies will be increasingly used to analyze complex DBPs produced in different treatment processes with the aim to identify potential drivers of toxicity.
