Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory...

Autores
Fernandez, Jose Luis; Zoski, Cynthia
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Mechanistic studies of the hydrogen evolution reaction (HER) on nanoelectrode ensembles of ultramicroelectrode dimensions (UME-NEEs) are demonstrated using addressable nanoelectrode membrane arrays (ANEMAs). A kinetic model considering simultaneous occurrence of all elementary steps and the effects of mass transport to/from the UME-NEE surface was developed and used to interpret HER steady-state voltammograms (SSVs). The analysis accounts for the effect of fraction of covered area, f, and roughness factor, fR, of the nanoelectrodes on HER SSVs and illustrates the roles of these parameters in mechanistic studies of electrocatalyzed multistep reactions on UME-NEEs. The behavior of bare Au UME-NEEs was studied in acid solution, and characterization of the HER on these electrodes was performed by SSV and scanning electrochemical microscopy (SECM) in the substrate generation-tip collection mode (SG-TC). The activity of Au NEEs for the HER was found to be similar to that of macrosized polycrystalline Au. Selective electrodeposition of Pt NPs was performed on Au UME-NEEs, and SSV was used to study the kinetic mechanism of the HER in acid on the Pt-modified UME-NEEs with different f values. UME-NEEs with excess Pt showed HER activity equivalent to polycrystalline Pt, while those with small, almost undetectable, amounts of Pt showed HER behavior that could not be explained as the addition of pure Au and pure Pt contributions. SECM activity screening on Pt-modified ANEMAs detected changes in the apparent electrocatalytic activity for the HER, in agreement with corresponding SSVs.
Fil: Fernandez, Jose Luis. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; Argentina. Universidad Nacional del Litoral. Facultad de Ingeniería Química. Programa de Electroquímica Aplicada e Ingeniería Electroquímica; Argentina
Fil: Zoski, Cynthia. New Mexico State University; Estados Unidos
Materia
HYDROGEN EVOLUTION REACTION
NANOELECTRODE ENSEMBLES
NANOPARTICLES
ARRAY ELECTRODES
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/89465
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/89465
network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and ExperimentFernandez, Jose LuisZoski, CynthiaHYDROGEN EVOLUTION REACTIONNANOELECTRODE ENSEMBLESNANOPARTICLESARRAY ELECTRODEShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Mechanistic studies of the hydrogen evolution reaction (HER) on nanoelectrode ensembles of ultramicroelectrode dimensions (UME-NEEs) are demonstrated using addressable nanoelectrode membrane arrays (ANEMAs). A kinetic model considering simultaneous occurrence of all elementary steps and the effects of mass transport to/from the UME-NEE surface was developed and used to interpret HER steady-state voltammograms (SSVs). The analysis accounts for the effect of fraction of covered area, f, and roughness factor, fR, of the nanoelectrodes on HER SSVs and illustrates the roles of these parameters in mechanistic studies of electrocatalyzed multistep reactions on UME-NEEs. The behavior of bare Au UME-NEEs was studied in acid solution, and characterization of the HER on these electrodes was performed by SSV and scanning electrochemical microscopy (SECM) in the substrate generation-tip collection mode (SG-TC). The activity of Au NEEs for the HER was found to be similar to that of macrosized polycrystalline Au. Selective electrodeposition of Pt NPs was performed on Au UME-NEEs, and SSV was used to study the kinetic mechanism of the HER in acid on the Pt-modified UME-NEEs with different f values. UME-NEEs with excess Pt showed HER activity equivalent to polycrystalline Pt, while those with small, almost undetectable, amounts of Pt showed HER behavior that could not be explained as the addition of pure Au and pure Pt contributions. SECM activity screening on Pt-modified ANEMAs detected changes in the apparent electrocatalytic activity for the HER, in agreement with corresponding SSVs.Fil: Fernandez, Jose Luis. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; Argentina. Universidad Nacional del Litoral. Facultad de Ingeniería Química. Programa de Electroquímica Aplicada e Ingeniería Electroquímica; ArgentinaFil: Zoski, Cynthia. New Mexico State University; Estados UnidosAmerican Chemical Society2018-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/89465Fernandez, Jose Luis; Zoski, Cynthia; Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment; American Chemical Society; Journal of Physical Chemistry C; 122; 1; 1-2018; 71-821932-7447CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.7b08976info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpcc.7b08976info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:16:30Zoai:ri.conicet.gov.ar:11336/89465instacron: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 15:16:30.374CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
title Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
spellingShingle Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
Fernandez, Jose Luis
HYDROGEN EVOLUTION REACTION
NANOELECTRODE ENSEMBLES
NANOPARTICLES
ARRAY ELECTRODES
title_short Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
title_full Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
title_fullStr Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
title_full_unstemmed Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
title_sort Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment
dc.creator.none.fl_str_mv Fernandez, Jose Luis
Zoski, Cynthia
author Fernandez, Jose Luis
author_facet Fernandez, Jose Luis
Zoski, Cynthia
author_role author
author2 Zoski, Cynthia
author2_role author
dc.subject.none.fl_str_mv HYDROGEN EVOLUTION REACTION
NANOELECTRODE ENSEMBLES
NANOPARTICLES
ARRAY ELECTRODES
topic HYDROGEN EVOLUTION REACTION
NANOELECTRODE ENSEMBLES
NANOPARTICLES
ARRAY ELECTRODES
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Mechanistic studies of the hydrogen evolution reaction (HER) on nanoelectrode ensembles of ultramicroelectrode dimensions (UME-NEEs) are demonstrated using addressable nanoelectrode membrane arrays (ANEMAs). A kinetic model considering simultaneous occurrence of all elementary steps and the effects of mass transport to/from the UME-NEE surface was developed and used to interpret HER steady-state voltammograms (SSVs). The analysis accounts for the effect of fraction of covered area, f, and roughness factor, fR, of the nanoelectrodes on HER SSVs and illustrates the roles of these parameters in mechanistic studies of electrocatalyzed multistep reactions on UME-NEEs. The behavior of bare Au UME-NEEs was studied in acid solution, and characterization of the HER on these electrodes was performed by SSV and scanning electrochemical microscopy (SECM) in the substrate generation-tip collection mode (SG-TC). The activity of Au NEEs for the HER was found to be similar to that of macrosized polycrystalline Au. Selective electrodeposition of Pt NPs was performed on Au UME-NEEs, and SSV was used to study the kinetic mechanism of the HER in acid on the Pt-modified UME-NEEs with different f values. UME-NEEs with excess Pt showed HER activity equivalent to polycrystalline Pt, while those with small, almost undetectable, amounts of Pt showed HER behavior that could not be explained as the addition of pure Au and pure Pt contributions. SECM activity screening on Pt-modified ANEMAs detected changes in the apparent electrocatalytic activity for the HER, in agreement with corresponding SSVs.
Fil: Fernandez, Jose Luis. Universidad Nacional del Litoral. Instituto de Química Aplicada del Litoral. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Química Aplicada del Litoral.; Argentina. Universidad Nacional del Litoral. Facultad de Ingeniería Química. Programa de Electroquímica Aplicada e Ingeniería Electroquímica; Argentina
Fil: Zoski, Cynthia. New Mexico State University; Estados Unidos
description Mechanistic studies of the hydrogen evolution reaction (HER) on nanoelectrode ensembles of ultramicroelectrode dimensions (UME-NEEs) are demonstrated using addressable nanoelectrode membrane arrays (ANEMAs). A kinetic model considering simultaneous occurrence of all elementary steps and the effects of mass transport to/from the UME-NEE surface was developed and used to interpret HER steady-state voltammograms (SSVs). The analysis accounts for the effect of fraction of covered area, f, and roughness factor, fR, of the nanoelectrodes on HER SSVs and illustrates the roles of these parameters in mechanistic studies of electrocatalyzed multistep reactions on UME-NEEs. The behavior of bare Au UME-NEEs was studied in acid solution, and characterization of the HER on these electrodes was performed by SSV and scanning electrochemical microscopy (SECM) in the substrate generation-tip collection mode (SG-TC). The activity of Au NEEs for the HER was found to be similar to that of macrosized polycrystalline Au. Selective electrodeposition of Pt NPs was performed on Au UME-NEEs, and SSV was used to study the kinetic mechanism of the HER in acid on the Pt-modified UME-NEEs with different f values. UME-NEEs with excess Pt showed HER activity equivalent to polycrystalline Pt, while those with small, almost undetectable, amounts of Pt showed HER behavior that could not be explained as the addition of pure Au and pure Pt contributions. SECM activity screening on Pt-modified ANEMAs detected changes in the apparent electrocatalytic activity for the HER, in agreement with corresponding SSVs.
publishDate 2018
dc.date.none.fl_str_mv 2018-01
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/11336/89465
Fernandez, Jose Luis; Zoski, Cynthia; Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment; American Chemical Society; Journal of Physical Chemistry C; 122; 1; 1-2018; 71-82
1932-7447
CONICET Digital
CONICET
url http://hdl.handle.net/11336/89465
identifier_str_mv Fernandez, Jose Luis; Zoski, Cynthia; Voltammetric and Scanning Electrochemical Microscopy Investigations of the Hydrogen Evolution Reaction in Acid at Nanostructured Ensembles of Ultramicroelectrode Dimensions: Theory and Experiment; American Chemical Society; Journal of Physical Chemistry C; 122; 1; 1-2018; 71-82
1932-7447
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.7b08976
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpcc.7b08976
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
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: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 13.22299

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