Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases

Dielectric barrier discharge ionization has gained significant interest due to its versatility and broad chemical coverage. Although electrospray ionization (ESI) is the most commonly used ionization source for organic contaminant analysis by liquid chromatography–mass spectrometry (LC–MS), it has l...

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Autores: Caño-Carrillo, Irene, Gilbert-López, Bienvenida, Moreno-González, David, Franzke, Joachim, García-Reyes, Juan F.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2025
País:España
Institución:Universidad de Jaén
Repositorio:RUJA. Repositorio Institucional de la Producción Científica de la Universidad de Jaén
OAI Identifier:oai:ruja.ujaen.es:10953/6314
Acceso en línea:https://doi.org/10.1021/acs.analchem.5c03745
https://hdl.handle.net/10953/6314
Access Level:acceso abierto
Palabra clave:Liquid chromatography, mass spectrometry, ionization source, organic contaminants
2301.03
2301.10
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spelling Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gasesCaño-Carrillo, IreneGilbert-López, BienvenidaMoreno-González, DavidFranzke, JoachimGarcía-Reyes, Juan F.Liquid chromatography, mass spectrometry, ionization source, organic contaminants2301.032301.10Dielectric barrier discharge ionization has gained significant interest due to its versatility and broad chemical coverage. Although electrospray ionization (ESI) is the most commonly used ionization source for organic contaminant analysis by liquid chromatography–mass spectrometry (LC–MS), it has limitations such as low ionization efficiency for nonpolar compounds and matrix effects. This study investigates the potential of flexible microtube plasma (FμTP) as an alternative ionization source for the LC–MS determination of multiclass pesticides comprising ESI-amenable and organochlorine contaminants. The analytical performance of FμTP was assessed in terms of limits of quantification, reproducibility, linearity, and matrix effects, comparing the results to those obtained with ESI and atmospheric pressure chemical ionization (APCI) sources. Sensitivity assessment based on calibration slopes showed that 70% of the pesticides had higher sensitivity with FμTP than with ESI. Regarding the matrix effects, between 76 and 86% of the pesticides showed negligible matrix effects for FμTP, compared to 35–67% for ESI and 55–75% for APCI across the different matrices evaluated. The study further explored the use of argon and argon–propane mixtures as alternatives to helium as discharge gases. Results showed similar LOQs for nearly 90% of the pesticides in the positive mode and 80% of the organochlorines in the negative mode. Notably, some ion species differed when using argon-based gases for certain organochlorine pesticides, suggesting the discharge gas influences the ionization mechanism, especially in the negative mode. Overall, FμTP proves to be a sensitive and robust miniaturized ionization source, expanding the chemical space and making it useful for both target and nontarget screening applications.American Chemical Society202520252025info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfapplication/pdfhttps://doi.org/10.1021/acs.analchem.5c03745https://hdl.handle.net/10953/6314reponame:RUJA. Repositorio Institucional de la Producción Científica de la Universidad de Jaéninstname:Universidad de JaénInglésAnalytical Chemistry (2025) 97, 38, 20962-20972Attribution-NonCommercial-NoDerivs 3.0 Spainhttp://creativecommons.org/licenses/by-nc-nd/3.0/es/info:eu-repo/semantics/openAccessoai:ruja.ujaen.es:10953/63142026-06-24T12:41:07Z
dc.title.none.fl_str_mv Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
title Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
spellingShingle Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
Caño-Carrillo, Irene
Liquid chromatography, mass spectrometry, ionization source, organic contaminants
2301.03
2301.10
title_short Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
title_full Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
title_fullStr Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
title_full_unstemmed Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
title_sort Efficient and wide chemical-space ionization of organic contaminants using LC-MS with a miniaturized plasma source applying different discharge gases
dc.creator.none.fl_str_mv Caño-Carrillo, Irene
Gilbert-López, Bienvenida
Moreno-González, David
Franzke, Joachim
García-Reyes, Juan F.
author Caño-Carrillo, Irene
author_facet Caño-Carrillo, Irene
Gilbert-López, Bienvenida
Moreno-González, David
Franzke, Joachim
García-Reyes, Juan F.
author_role author
author2 Gilbert-López, Bienvenida
Moreno-González, David
Franzke, Joachim
García-Reyes, Juan F.
author2_role author
author
author
author
dc.subject.none.fl_str_mv Liquid chromatography, mass spectrometry, ionization source, organic contaminants
2301.03
2301.10
topic Liquid chromatography, mass spectrometry, ionization source, organic contaminants
2301.03
2301.10
description Dielectric barrier discharge ionization has gained significant interest due to its versatility and broad chemical coverage. Although electrospray ionization (ESI) is the most commonly used ionization source for organic contaminant analysis by liquid chromatography–mass spectrometry (LC–MS), it has limitations such as low ionization efficiency for nonpolar compounds and matrix effects. This study investigates the potential of flexible microtube plasma (FμTP) as an alternative ionization source for the LC–MS determination of multiclass pesticides comprising ESI-amenable and organochlorine contaminants. The analytical performance of FμTP was assessed in terms of limits of quantification, reproducibility, linearity, and matrix effects, comparing the results to those obtained with ESI and atmospheric pressure chemical ionization (APCI) sources. Sensitivity assessment based on calibration slopes showed that 70% of the pesticides had higher sensitivity with FμTP than with ESI. Regarding the matrix effects, between 76 and 86% of the pesticides showed negligible matrix effects for FμTP, compared to 35–67% for ESI and 55–75% for APCI across the different matrices evaluated. The study further explored the use of argon and argon–propane mixtures as alternatives to helium as discharge gases. Results showed similar LOQs for nearly 90% of the pesticides in the positive mode and 80% of the organochlorines in the negative mode. Notably, some ion species differed when using argon-based gases for certain organochlorine pesticides, suggesting the discharge gas influences the ionization mechanism, especially in the negative mode. Overall, FμTP proves to be a sensitive and robust miniaturized ionization source, expanding the chemical space and making it useful for both target and nontarget screening applications.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://doi.org/10.1021/acs.analchem.5c03745
https://hdl.handle.net/10953/6314
url https://doi.org/10.1021/acs.analchem.5c03745
https://hdl.handle.net/10953/6314
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Analytical Chemistry (2025) 97, 38, 20962-20972
dc.rights.none.fl_str_mv Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:RUJA. Repositorio Institucional de la Producción Científica de la Universidad de Jaén
instname:Universidad de Jaén
instname_str Universidad de Jaén
reponame_str RUJA. Repositorio Institucional de la Producción Científica de la Universidad de Jaén
collection RUJA. Repositorio Institucional de la Producción Científica de la Universidad de Jaén
repository.name.fl_str_mv
repository.mail.fl_str_mv
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