Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media

Autores
Hötger, Diana; Etzkorn, Markus; Morchutt, Claudius; Wurster, Benjamin; Dreiser, Jan; Stepanow, Sebastian; Grumelli, Doris Elda; Gutzler, Rico; Kern, Klaus
Año de publicación
2019
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Transition metal atoms stabilised by organic ligands or as oxides exhibit promising catalytic activity for the electrocatalytic reduction and evolution of oxygen. Built-up from earth-abundant elements, they offer affordable alternatives to precious-metal based catalysts for application in fuel cells and electrolysers. For the understanding of a catalyst's activity, insight into its structure on the atomic scale is of highest importance, yet commonly challenging to experimentally access. Here, the structural integrity of a bimetallic iron tetrapyridylporphyrin with co-adsorbed cobalt electrocatalyst on Au(111) is investigated using scanning tunneling microscopy and X-ray absorption spectroscopy. Topographic and spectroscopic characterization reveals structural changes of the molecular coordination network after oxygen reduction, and its decomposition and transformation into catalytically active Co/Fe (oxyhydr)oxide during oxygen evolution. The data establishes a structure–property relationship for the catalyst as a function of electrochemical potential and, in addition, highlights how the reaction direction of electrochemical interconversion between molecular oxygen and hydroxyl anions can have very different effects on the catalyst's structure.
Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas
Materia
Química
Catalysts
Macrocyclic molecules
Nivel de accesibilidad
acceso abierto
Condiciones de uso
http://creativecommons.org/licenses/by-nc-sa/4.0/
Repositorio
SEDICI (UNLP)
Institución
Universidad Nacional de La Plata
OAI Identificador
oai:sedici.unlp.edu.ar:10915/132485
Acceder
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network_name_str SEDICI (UNLP)
spelling Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline mediaHötger, DianaEtzkorn, MarkusMorchutt, ClaudiusWurster, BenjaminDreiser, JanStepanow, SebastianGrumelli, Doris EldaGutzler, RicoKern, KlausQuímicaCatalystsMacrocyclic moleculesTransition metal atoms stabilised by organic ligands or as oxides exhibit promising catalytic activity for the electrocatalytic reduction and evolution of oxygen. Built-up from earth-abundant elements, they offer affordable alternatives to precious-metal based catalysts for application in fuel cells and electrolysers. For the understanding of a catalyst's activity, insight into its structure on the atomic scale is of highest importance, yet commonly challenging to experimentally access. Here, the structural integrity of a bimetallic iron tetrapyridylporphyrin with co-adsorbed cobalt electrocatalyst on Au(111) is investigated using scanning tunneling microscopy and X-ray absorption spectroscopy. Topographic and spectroscopic characterization reveals structural changes of the molecular coordination network after oxygen reduction, and its decomposition and transformation into catalytically active Co/Fe (oxyhydr)oxide during oxygen evolution. The data establishes a structure–property relationship for the catalyst as a function of electrochemical potential and, in addition, highlights how the reaction direction of electrochemical interconversion between molecular oxygen and hydroxyl anions can have very different effects on the catalyst's structure.Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas2019info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionArticulohttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdf2587-2594http://sedici.unlp.edu.ar/handle/10915/132485enginfo:eu-repo/semantics/altIdentifier/issn/1463-9084info:eu-repo/semantics/altIdentifier/issn/1463-9076info:eu-repo/semantics/altIdentifier/doi/10.1039/c8cp07463ainfo:eu-repo/semantics/altIdentifier/pmid/30657498info:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc-sa/4.0/Creative Commons Attribution-NonCommercial-ShareAlike 4.0 International (CC BY-NC-SA 4.0)reponame:SEDICI (UNLP)instname:Universidad Nacional de La Platainstacron:UNLP2025-09-03T11:04:18Zoai:sedici.unlp.edu.ar:10915/132485Institucionalhttp://sedici.unlp.edu.ar/Universidad públicaNo correspondehttp://sedici.unlp.edu.ar/oai/snrdalira@sedici.unlp.edu.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:13292025-09-03 11:04:18.514SEDICI (UNLP) - Universidad Nacional de La Platafalse
dc.title.none.fl_str_mv Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
title Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
spellingShingle Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
Hötger, Diana
Química
Catalysts
Macrocyclic molecules
title_short Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
title_full Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
title_fullStr Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
title_full_unstemmed Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
title_sort Stability of metallo-porphyrin networks under oxygen reduction and evolution conditions in alkaline media
dc.creator.none.fl_str_mv Hötger, Diana
Etzkorn, Markus
Morchutt, Claudius
Wurster, Benjamin
Dreiser, Jan
Stepanow, Sebastian
Grumelli, Doris Elda
Gutzler, Rico
Kern, Klaus
author Hötger, Diana
author_facet Hötger, Diana
Etzkorn, Markus
Morchutt, Claudius
Wurster, Benjamin
Dreiser, Jan
Stepanow, Sebastian
Grumelli, Doris Elda
Gutzler, Rico
Kern, Klaus
author_role author
author2 Etzkorn, Markus
Morchutt, Claudius
Wurster, Benjamin
Dreiser, Jan
Stepanow, Sebastian
Grumelli, Doris Elda
Gutzler, Rico
Kern, Klaus
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Química
Catalysts
Macrocyclic molecules
topic Química
Catalysts
Macrocyclic molecules
dc.description.none.fl_txt_mv Transition metal atoms stabilised by organic ligands or as oxides exhibit promising catalytic activity for the electrocatalytic reduction and evolution of oxygen. Built-up from earth-abundant elements, they offer affordable alternatives to precious-metal based catalysts for application in fuel cells and electrolysers. For the understanding of a catalyst's activity, insight into its structure on the atomic scale is of highest importance, yet commonly challenging to experimentally access. Here, the structural integrity of a bimetallic iron tetrapyridylporphyrin with co-adsorbed cobalt electrocatalyst on Au(111) is investigated using scanning tunneling microscopy and X-ray absorption spectroscopy. Topographic and spectroscopic characterization reveals structural changes of the molecular coordination network after oxygen reduction, and its decomposition and transformation into catalytically active Co/Fe (oxyhydr)oxide during oxygen evolution. The data establishes a structure–property relationship for the catalyst as a function of electrochemical potential and, in addition, highlights how the reaction direction of electrochemical interconversion between molecular oxygen and hydroxyl anions can have very different effects on the catalyst's structure.
Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas
description Transition metal atoms stabilised by organic ligands or as oxides exhibit promising catalytic activity for the electrocatalytic reduction and evolution of oxygen. Built-up from earth-abundant elements, they offer affordable alternatives to precious-metal based catalysts for application in fuel cells and electrolysers. For the understanding of a catalyst's activity, insight into its structure on the atomic scale is of highest importance, yet commonly challenging to experimentally access. Here, the structural integrity of a bimetallic iron tetrapyridylporphyrin with co-adsorbed cobalt electrocatalyst on Au(111) is investigated using scanning tunneling microscopy and X-ray absorption spectroscopy. Topographic and spectroscopic characterization reveals structural changes of the molecular coordination network after oxygen reduction, and its decomposition and transformation into catalytically active Co/Fe (oxyhydr)oxide during oxygen evolution. The data establishes a structure–property relationship for the catalyst as a function of electrochemical potential and, in addition, highlights how the reaction direction of electrochemical interconversion between molecular oxygen and hydroxyl anions can have very different effects on the catalyst's structure.
publishDate 2019
dc.date.none.fl_str_mv 2019
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
Articulo
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://sedici.unlp.edu.ar/handle/10915/132485
url http://sedici.unlp.edu.ar/handle/10915/132485
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/issn/1463-9084
info:eu-repo/semantics/altIdentifier/issn/1463-9076
info:eu-repo/semantics/altIdentifier/doi/10.1039/c8cp07463a
info:eu-repo/semantics/altIdentifier/pmid/30657498
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by-nc-sa/4.0/
Creative Commons Attribution-NonCommercial-ShareAlike 4.0 International (CC BY-NC-SA 4.0)
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by-nc-sa/4.0/
Creative Commons Attribution-NonCommercial-ShareAlike 4.0 International (CC BY-NC-SA 4.0)
dc.format.none.fl_str_mv application/pdf
2587-2594
dc.source.none.fl_str_mv reponame:SEDICI (UNLP)
instname:Universidad Nacional de La Plata
instacron:UNLP
reponame_str SEDICI (UNLP)
collection SEDICI (UNLP)
instname_str Universidad Nacional de La Plata
instacron_str UNLP
institution UNLP
repository.name.fl_str_mv SEDICI (UNLP) - Universidad Nacional de La Plata
repository.mail.fl_str_mv alira@sedici.unlp.edu.ar
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score 13.13397

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