Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows

Dissolved organic matter (DOM) in aquatic systems is a highly heterogeneous mixture of water-soluble organic compounds, acting as a major carbon reservoir driving biogeochemical cycles. Understanding DOM molecular composition is thus of vital interest for the health assessment of aquatic ecosystems,...

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Autores: Patrone, Jessica, Vila-Costa, Maria, Dachs, Jordi, Papazian, Stefano, Gago-Ferrero, Pablo, Gil-Solsona, Rubén
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/363844
Acceso en línea:http://hdl.handle.net/10261/363844
https://api.elsevier.com/content/abstract/scopus_id/85197537458
Access Level:acceso abierto
Palabra clave:Molecular fingerprinting
LC-orbitrap
Dissolved organic matter
Environmental water
http://metadata.un.org/sdg/6
Ensure availability and sustainable management of water and sanitation for all
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spelling Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted WorkflowsPatrone, JessicaVila-Costa, MariaDachs, JordiPapazian, StefanoGago-Ferrero, PabloGil-Solsona, RubénMolecular fingerprintingLC-orbitrapDissolved organic matterEnvironmental waterhttp://metadata.un.org/sdg/6Ensure availability and sustainable management of water and sanitation for allDissolved organic matter (DOM) in aquatic systems is a highly heterogeneous mixture of water-soluble organic compounds, acting as a major carbon reservoir driving biogeochemical cycles. Understanding DOM molecular composition is thus of vital interest for the health assessment of aquatic ecosystems, yet its characterization poses challenges due to its complex and dynamic chemical profile. Here, we performed a comprehensive chemical analysis of DOM from highly urbanized river and seawater sources and compared it to drinking water. Extensive analyses by nontargeted direct infusion (DI) and liquid chromatography (LC) high-resolution mass spectrometry (HRMS) through Orbitrap were integrated with novel computational workflows to allow molecular- and structural-level characterization of DOM. Across all water samples, over 7000 molecular formulas were calculated using both methods (∼4200 in DI and ∼3600 in LC). While the DI approach was limited to molecular formula calculation, the downstream data processing of MS2 spectral information combining library matching and in silico predictions enabled a comprehensive structural-level characterization of 16% of the molecular space detected by LC-HRMS across all water samples. Both analytical methods proved complementary, covering a broad chemical space that includes more highly polar compounds with DI and more less polar ones with LC. The innovative integration of diverse analytical techniques and computational workflow introduces a robust and largely available framework in the field, providing a widely applicable approach that significantly contributes to understanding the complex molecular composition of DOM.This work was supported by the Spanish Ministry of Science and Innovation through the projects LINKAGES and PLANKTONPOPs included in Severo Ochoa Excellence Program (CEX2018-000794-S), and through project MIQAS (PID2021-128084OB-I00). Dr. Núria Catalán and Jeffrey A. Hawkes are acknowledged for the R code used in DI data treatment. The research group of Global Change and Genomic Biogeochemistry receives support from the Catalan Government (2017SGR800). IDAEA-CSIC is a Centre of Excellence Severo Ochoa (Spanish Ministry of Science and Innovation, Project CEX2018-000794-S).Peer reviewedAmerican Chemical Society0009-0008-0953-31250000-0003-1730-84180000-0002-4237-169X0000-0003-2538-87020000-0002-5987-03990000-0002-4269-1036Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202420242024info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/363844https://api.elsevier.com/content/abstract/scopus_id/85197537458reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)InglésEnvironmental science & technologyhttps://doi.org/10.1021/acs.est.4c00876Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3638442026-05-22T06:33:51Z
dc.title.none.fl_str_mv Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
title Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
spellingShingle Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
Patrone, Jessica
Molecular fingerprinting
LC-orbitrap
Dissolved organic matter
Environmental water
http://metadata.un.org/sdg/6
Ensure availability and sustainable management of water and sanitation for all
title_short Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
title_full Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
title_fullStr Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
title_full_unstemmed Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
title_sort Enhancing Molecular Characterization of Dissolved Organic Matter by Integrative Direct Infusion and Liquid Chromatography Nontargeted Workflows
dc.creator.none.fl_str_mv Patrone, Jessica
Vila-Costa, Maria
Dachs, Jordi
Papazian, Stefano
Gago-Ferrero, Pablo
Gil-Solsona, Rubén
author Patrone, Jessica
author_facet Patrone, Jessica
Vila-Costa, Maria
Dachs, Jordi
Papazian, Stefano
Gago-Ferrero, Pablo
Gil-Solsona, Rubén
author_role author
author2 Vila-Costa, Maria
Dachs, Jordi
Papazian, Stefano
Gago-Ferrero, Pablo
Gil-Solsona, Rubén
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv 0009-0008-0953-3125
0000-0003-1730-8418
0000-0002-4237-169X
0000-0003-2538-8702
0000-0002-5987-0399
0000-0002-4269-1036
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Molecular fingerprinting
LC-orbitrap
Dissolved organic matter
Environmental water
http://metadata.un.org/sdg/6
Ensure availability and sustainable management of water and sanitation for all
topic Molecular fingerprinting
LC-orbitrap
Dissolved organic matter
Environmental water
http://metadata.un.org/sdg/6
Ensure availability and sustainable management of water and sanitation for all
description Dissolved organic matter (DOM) in aquatic systems is a highly heterogeneous mixture of water-soluble organic compounds, acting as a major carbon reservoir driving biogeochemical cycles. Understanding DOM molecular composition is thus of vital interest for the health assessment of aquatic ecosystems, yet its characterization poses challenges due to its complex and dynamic chemical profile. Here, we performed a comprehensive chemical analysis of DOM from highly urbanized river and seawater sources and compared it to drinking water. Extensive analyses by nontargeted direct infusion (DI) and liquid chromatography (LC) high-resolution mass spectrometry (HRMS) through Orbitrap were integrated with novel computational workflows to allow molecular- and structural-level characterization of DOM. Across all water samples, over 7000 molecular formulas were calculated using both methods (∼4200 in DI and ∼3600 in LC). While the DI approach was limited to molecular formula calculation, the downstream data processing of MS2 spectral information combining library matching and in silico predictions enabled a comprehensive structural-level characterization of 16% of the molecular space detected by LC-HRMS across all water samples. Both analytical methods proved complementary, covering a broad chemical space that includes more highly polar compounds with DI and more less polar ones with LC. The innovative integration of diverse analytical techniques and computational workflow introduces a robust and largely available framework in the field, providing a widely applicable approach that significantly contributes to understanding the complex molecular composition of DOM.
publishDate 2024
dc.date.none.fl_str_mv 2024
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/363844
https://api.elsevier.com/content/abstract/scopus_id/85197537458
url http://hdl.handle.net/10261/363844
https://api.elsevier.com/content/abstract/scopus_id/85197537458
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Environmental science & technology
https://doi.org/10.1021/acs.est.4c00876
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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