Theresa Guillette, Whitney Stutts, Andrew Baumeister, David Liles, Theresa Olechiw, Johnsie Lang
{"title":"稳定土核中全氟烷基和多氟烷基物质(PFAS)的红外基质辅助激光解吸电喷雾电离(IR-MALDESI)质谱成像","authors":"Theresa Guillette, Whitney Stutts, Andrew Baumeister, David Liles, Theresa Olechiw, Johnsie Lang","doi":"10.1021/jasms.4c00428","DOIUrl":null,"url":null,"abstract":"<p><p>Infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) was coupled with high-resolution accurate-mass-mass spectrometry (HRAM-MS) to image perfluoroalkyl and polyfluoroalkyl substances (PFAS) in stabilized soil cores. Previous field-scale research demonstrated a substantial decrease in the leachability of PFAS following the application of in situ stabilization and solidification (S/S) in an aqueous film-forming foam (AFFF) source zone. While this previous study empirically confirmed the effectiveness of S/S, there was no definitive identification of the operative retention mechanisms. Therefore, the objective of this follow-on study was to (1) develop a high-resolution mass spectrometry-based imaging technique for PFAS on stabilized and background control soil cores and (2) determine if chemical characteristics of the amendments were associated spatially with the PFAS distribution within the soil cores at a micrometer scale. Intact frozen soil cores were imaged in negative ion mode, targeted and suspect screening analyses were conducted, features were identified using suspect lists, and analytes were presented as raw abundances matched against several databases. IR-MALDESI imaging results confirmed the colocation of PFOS and PFHxS with non-PFAS chemical features (e.g., mono- and diglycerides) associated with treatments including amendments, which suggests chemical fixation as a mechanism of stabilization for PFAS in stabilized soil cores.</p>","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"653-657"},"PeriodicalIF":3.1000,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Infrared Matrix-Assisted Laser Desorption Electrospray Ionization (IR-MALDESI) Mass Spectrometry Imaging of Per- and Polyfluoroalkyl Substances (PFAS) in Stabilized Soil Cores.\",\"authors\":\"Theresa Guillette, Whitney Stutts, Andrew Baumeister, David Liles, Theresa Olechiw, Johnsie Lang\",\"doi\":\"10.1021/jasms.4c00428\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) was coupled with high-resolution accurate-mass-mass spectrometry (HRAM-MS) to image perfluoroalkyl and polyfluoroalkyl substances (PFAS) in stabilized soil cores. Previous field-scale research demonstrated a substantial decrease in the leachability of PFAS following the application of in situ stabilization and solidification (S/S) in an aqueous film-forming foam (AFFF) source zone. While this previous study empirically confirmed the effectiveness of S/S, there was no definitive identification of the operative retention mechanisms. Therefore, the objective of this follow-on study was to (1) develop a high-resolution mass spectrometry-based imaging technique for PFAS on stabilized and background control soil cores and (2) determine if chemical characteristics of the amendments were associated spatially with the PFAS distribution within the soil cores at a micrometer scale. Intact frozen soil cores were imaged in negative ion mode, targeted and suspect screening analyses were conducted, features were identified using suspect lists, and analytes were presented as raw abundances matched against several databases. IR-MALDESI imaging results confirmed the colocation of PFOS and PFHxS with non-PFAS chemical features (e.g., mono- and diglycerides) associated with treatments including amendments, which suggests chemical fixation as a mechanism of stabilization for PFAS in stabilized soil cores.</p>\",\"PeriodicalId\":672,\"journal\":{\"name\":\"Journal of the American Society for Mass Spectrometry\",\"volume\":\" \",\"pages\":\"653-657\"},\"PeriodicalIF\":3.1000,\"publicationDate\":\"2025-04-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Society for Mass Spectrometry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jasms.4c00428\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/3/18 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"BIOCHEMICAL RESEARCH METHODS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Society for Mass Spectrometry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jasms.4c00428","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/3/18 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"BIOCHEMICAL RESEARCH METHODS","Score":null,"Total":0}
Infrared Matrix-Assisted Laser Desorption Electrospray Ionization (IR-MALDESI) Mass Spectrometry Imaging of Per- and Polyfluoroalkyl Substances (PFAS) in Stabilized Soil Cores.
Infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) was coupled with high-resolution accurate-mass-mass spectrometry (HRAM-MS) to image perfluoroalkyl and polyfluoroalkyl substances (PFAS) in stabilized soil cores. Previous field-scale research demonstrated a substantial decrease in the leachability of PFAS following the application of in situ stabilization and solidification (S/S) in an aqueous film-forming foam (AFFF) source zone. While this previous study empirically confirmed the effectiveness of S/S, there was no definitive identification of the operative retention mechanisms. Therefore, the objective of this follow-on study was to (1) develop a high-resolution mass spectrometry-based imaging technique for PFAS on stabilized and background control soil cores and (2) determine if chemical characteristics of the amendments were associated spatially with the PFAS distribution within the soil cores at a micrometer scale. Intact frozen soil cores were imaged in negative ion mode, targeted and suspect screening analyses were conducted, features were identified using suspect lists, and analytes were presented as raw abundances matched against several databases. IR-MALDESI imaging results confirmed the colocation of PFOS and PFHxS with non-PFAS chemical features (e.g., mono- and diglycerides) associated with treatments including amendments, which suggests chemical fixation as a mechanism of stabilization for PFAS in stabilized soil cores.
期刊介绍:
The Journal of the American Society for Mass Spectrometry presents research papers covering all aspects of mass spectrometry, incorporating coverage of fields of scientific inquiry in which mass spectrometry can play a role.
Comprehensive in scope, the journal publishes papers on both fundamentals and applications of mass spectrometry. Fundamental subjects include instrumentation principles, design, and demonstration, structures and chemical properties of gas-phase ions, studies of thermodynamic properties, ion spectroscopy, chemical kinetics, mechanisms of ionization, theories of ion fragmentation, cluster ions, and potential energy surfaces. In addition to full papers, the journal offers Communications, Application Notes, and Accounts and Perspectives