Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge

Autores
Wibowo, Romualdus Enggar; Garcia Diez, Raul; Bystron, Tomas; van der Merwe, Marianne; Prokop, Martin; Arce, Mauricio Damián; Efimenko, Anna; Steigert, Alexander; Bernauer, Milan; Wilks, Regan G.; Bouzek, Karel; Bär, Marcus
Año de publicación
2024
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In situ tender X-ray absorption near-edge structure (XANES) spectroscopy at the P K-edge was utilized to investigate the oxidation mechanism of aqueous H3PO3 on Pt electrodes under various conditions relevant to high-temperature polymer electrolyte membrane fuel cell (HT-PEMFC) applications. XANES and electrochemical analysis were conducted under different tender X-ray irradiation doses, revealing that intense radiation induces the oxidation of aqueous H3PO3 via H2O yielding H3PO4 and H2. A broadly applicable experimental procedure was successfully developed to suppress these undesirable radiation-induced effects, enabling a more accurate determination of the aqueous H3PO3 oxidation mechanism. In situ XANES studies of aqueous 5 mol dm–3 H3PO3 on electrodes with varying Pt availability and surface roughness reveal that Pt catalyzes the oxidation of aqueous H3PO3 to H3PO4. This oxidation is enhanced upon applying a positive potential to the Pt electrode or raising the electrolyte temperature, the latter being corroborated by complementary ion-exchange chromatography measurements. Notably, all of these oxidation processes involve reactions with H2O, as further supported by XANES measurements of aqueous H3PO3 of different concentrations, showing a more pronounced oxidation in electrolytes with a higher H2O content. The significant role of water in the oxidation of H3PO3 to H3PO4 supports the reaction mechanisms proposed for various chemical processes observed in this work and provides valuable insights into potential strategies to mitigate Pt catalyst poisoning by H3PO3 during HT-PEMFC operation.
Fil: Wibowo, Romualdus Enggar. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Garcia Diez, Raul. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Bystron, Tomas. University of Chemistry and Technology Prague; República Checa
Fil: van der Merwe, Marianne. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Prokop, Martin. University Of Chemistry And Technology Prague; República Checa
Fil: Arce, Mauricio Damián. Comision Nacional de Energia Atomica. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. - Consejo Nacional de Investigaciones Cientificas y Tecnicas. Oficina de Coordinacion Administrativa Ciudad Universitaria. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia.; Argentina. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Efimenko, Anna. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Steigert, Alexander. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Bernauer, Milan. University Of Chemistry And Technology Prague; República Checa
Fil: Wilks, Regan G.. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Bouzek, Karel. University Of Chemistry And Technology Prague; República Checa
Fil: Bär, Marcus. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Materia
ELECTRODES
ELECTROLYTES
IRRADIATION
PLATINUM
X-RAY ABSORPTION NEAR EDGE SPECTROSCOPY
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/268142
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/268142
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -EdgeWibowo, Romualdus EnggarGarcia Diez, RaulBystron, Tomasvan der Merwe, MarianneProkop, MartinArce, Mauricio DamiánEfimenko, AnnaSteigert, AlexanderBernauer, MilanWilks, Regan G.Bouzek, KarelBär, MarcusELECTRODESELECTROLYTESIRRADIATIONPLATINUMX-RAY ABSORPTION NEAR EDGE SPECTROSCOPYhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1In situ tender X-ray absorption near-edge structure (XANES) spectroscopy at the P K-edge was utilized to investigate the oxidation mechanism of aqueous H3PO3 on Pt electrodes under various conditions relevant to high-temperature polymer electrolyte membrane fuel cell (HT-PEMFC) applications. XANES and electrochemical analysis were conducted under different tender X-ray irradiation doses, revealing that intense radiation induces the oxidation of aqueous H3PO3 via H2O yielding H3PO4 and H2. A broadly applicable experimental procedure was successfully developed to suppress these undesirable radiation-induced effects, enabling a more accurate determination of the aqueous H3PO3 oxidation mechanism. In situ XANES studies of aqueous 5 mol dm–3 H3PO3 on electrodes with varying Pt availability and surface roughness reveal that Pt catalyzes the oxidation of aqueous H3PO3 to H3PO4. This oxidation is enhanced upon applying a positive potential to the Pt electrode or raising the electrolyte temperature, the latter being corroborated by complementary ion-exchange chromatography measurements. Notably, all of these oxidation processes involve reactions with H2O, as further supported by XANES measurements of aqueous H3PO3 of different concentrations, showing a more pronounced oxidation in electrolytes with a higher H2O content. The significant role of water in the oxidation of H3PO3 to H3PO4 supports the reaction mechanisms proposed for various chemical processes observed in this work and provides valuable insights into potential strategies to mitigate Pt catalyst poisoning by H3PO3 during HT-PEMFC operation.Fil: Wibowo, Romualdus Enggar. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaFil: Garcia Diez, Raul. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaFil: Bystron, Tomas. University of Chemistry and Technology Prague; República ChecaFil: van der Merwe, Marianne. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaFil: Prokop, Martin. University Of Chemistry And Technology Prague; República ChecaFil: Arce, Mauricio Damián. Comision Nacional de Energia Atomica. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. - Consejo Nacional de Investigaciones Cientificas y Tecnicas. Oficina de Coordinacion Administrativa Ciudad Universitaria. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia.; Argentina. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaFil: Efimenko, Anna. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaFil: Steigert, Alexander. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaFil: Bernauer, Milan. University Of Chemistry And Technology Prague; República ChecaFil: Wilks, Regan G.. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaFil: Bouzek, Karel. University Of Chemistry And Technology Prague; República ChecaFil: Bär, Marcus. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; AlemaniaAmerican Chemical Society2024-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/268142Wibowo, Romualdus Enggar; Garcia Diez, Raul; Bystron, Tomas; van der Merwe, Marianne; Prokop, Martin; et al.; Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge; American Chemical Society; Journal of the American Chemical Society; 146; 11; 3-2024; 7386-73990002-7863CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/jacs.3c12381info:eu-repo/semantics/altIdentifier/doi/10.1021/jacs.3c12381info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:06:32Zoai:ri.conicet.gov.ar:11336/268142instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-15 15:06:32.416CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
title Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
spellingShingle Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
Wibowo, Romualdus Enggar
ELECTRODES
ELECTROLYTES
IRRADIATION
PLATINUM
X-RAY ABSORPTION NEAR EDGE SPECTROSCOPY
title_short Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
title_full Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
title_fullStr Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
title_full_unstemmed Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
title_sort Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge
dc.creator.none.fl_str_mv Wibowo, Romualdus Enggar
Garcia Diez, Raul
Bystron, Tomas
van der Merwe, Marianne
Prokop, Martin
Arce, Mauricio Damián
Efimenko, Anna
Steigert, Alexander
Bernauer, Milan
Wilks, Regan G.
Bouzek, Karel
Bär, Marcus
author Wibowo, Romualdus Enggar
author_facet Wibowo, Romualdus Enggar
Garcia Diez, Raul
Bystron, Tomas
van der Merwe, Marianne
Prokop, Martin
Arce, Mauricio Damián
Efimenko, Anna
Steigert, Alexander
Bernauer, Milan
Wilks, Regan G.
Bouzek, Karel
Bär, Marcus
author_role author
author2 Garcia Diez, Raul
Bystron, Tomas
van der Merwe, Marianne
Prokop, Martin
Arce, Mauricio Damián
Efimenko, Anna
Steigert, Alexander
Bernauer, Milan
Wilks, Regan G.
Bouzek, Karel
Bär, Marcus
author2_role author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv ELECTRODES
ELECTROLYTES
IRRADIATION
PLATINUM
X-RAY ABSORPTION NEAR EDGE SPECTROSCOPY
topic ELECTRODES
ELECTROLYTES
IRRADIATION
PLATINUM
X-RAY ABSORPTION NEAR EDGE SPECTROSCOPY
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv In situ tender X-ray absorption near-edge structure (XANES) spectroscopy at the P K-edge was utilized to investigate the oxidation mechanism of aqueous H3PO3 on Pt electrodes under various conditions relevant to high-temperature polymer electrolyte membrane fuel cell (HT-PEMFC) applications. XANES and electrochemical analysis were conducted under different tender X-ray irradiation doses, revealing that intense radiation induces the oxidation of aqueous H3PO3 via H2O yielding H3PO4 and H2. A broadly applicable experimental procedure was successfully developed to suppress these undesirable radiation-induced effects, enabling a more accurate determination of the aqueous H3PO3 oxidation mechanism. In situ XANES studies of aqueous 5 mol dm–3 H3PO3 on electrodes with varying Pt availability and surface roughness reveal that Pt catalyzes the oxidation of aqueous H3PO3 to H3PO4. This oxidation is enhanced upon applying a positive potential to the Pt electrode or raising the electrolyte temperature, the latter being corroborated by complementary ion-exchange chromatography measurements. Notably, all of these oxidation processes involve reactions with H2O, as further supported by XANES measurements of aqueous H3PO3 of different concentrations, showing a more pronounced oxidation in electrolytes with a higher H2O content. The significant role of water in the oxidation of H3PO3 to H3PO4 supports the reaction mechanisms proposed for various chemical processes observed in this work and provides valuable insights into potential strategies to mitigate Pt catalyst poisoning by H3PO3 during HT-PEMFC operation.
Fil: Wibowo, Romualdus Enggar. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Garcia Diez, Raul. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Bystron, Tomas. University of Chemistry and Technology Prague; República Checa
Fil: van der Merwe, Marianne. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Prokop, Martin. University Of Chemistry And Technology Prague; República Checa
Fil: Arce, Mauricio Damián. Comision Nacional de Energia Atomica. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. - Consejo Nacional de Investigaciones Cientificas y Tecnicas. Oficina de Coordinacion Administrativa Ciudad Universitaria. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia.; Argentina. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Efimenko, Anna. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Steigert, Alexander. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Bernauer, Milan. University Of Chemistry And Technology Prague; República Checa
Fil: Wilks, Regan G.. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
Fil: Bouzek, Karel. University Of Chemistry And Technology Prague; República Checa
Fil: Bär, Marcus. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH; Alemania
description In situ tender X-ray absorption near-edge structure (XANES) spectroscopy at the P K-edge was utilized to investigate the oxidation mechanism of aqueous H3PO3 on Pt electrodes under various conditions relevant to high-temperature polymer electrolyte membrane fuel cell (HT-PEMFC) applications. XANES and electrochemical analysis were conducted under different tender X-ray irradiation doses, revealing that intense radiation induces the oxidation of aqueous H3PO3 via H2O yielding H3PO4 and H2. A broadly applicable experimental procedure was successfully developed to suppress these undesirable radiation-induced effects, enabling a more accurate determination of the aqueous H3PO3 oxidation mechanism. In situ XANES studies of aqueous 5 mol dm–3 H3PO3 on electrodes with varying Pt availability and surface roughness reveal that Pt catalyzes the oxidation of aqueous H3PO3 to H3PO4. This oxidation is enhanced upon applying a positive potential to the Pt electrode or raising the electrolyte temperature, the latter being corroborated by complementary ion-exchange chromatography measurements. Notably, all of these oxidation processes involve reactions with H2O, as further supported by XANES measurements of aqueous H3PO3 of different concentrations, showing a more pronounced oxidation in electrolytes with a higher H2O content. The significant role of water in the oxidation of H3PO3 to H3PO4 supports the reaction mechanisms proposed for various chemical processes observed in this work and provides valuable insights into potential strategies to mitigate Pt catalyst poisoning by H3PO3 during HT-PEMFC operation.
publishDate 2024
dc.date.none.fl_str_mv 2024-03
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/268142
Wibowo, Romualdus Enggar; Garcia Diez, Raul; Bystron, Tomas; van der Merwe, Marianne; Prokop, Martin; et al.; Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge; American Chemical Society; Journal of the American Chemical Society; 146; 11; 3-2024; 7386-7399
0002-7863
CONICET Digital
CONICET
url http://hdl.handle.net/11336/268142
identifier_str_mv Wibowo, Romualdus Enggar; Garcia Diez, Raul; Bystron, Tomas; van der Merwe, Marianne; Prokop, Martin; et al.; Elucidating the Complex Oxidation Behavior of Aqueous H 3 PO 3 on Pt Electrodes via In Situ Tender X-ray Absorption Near-Edge Structure Spectroscopy at the P K -Edge; American Chemical Society; Journal of the American Chemical Society; 146; 11; 3-2024; 7386-7399
0002-7863
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/jacs.3c12381
info:eu-repo/semantics/altIdentifier/doi/10.1021/jacs.3c12381
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
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:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.221938

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