Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides

Autores
Sanchis Gual, Roger; Jaramillo Hernández, Camilo; Hunt, Diego; Seijas Da Silva, Álvaro; Mizrahi, Martin Daniel; Marini, Carlo; Oestreicher, Víctor Santiago Jesús; Abellán, Gonzalo
Año de publicación
2023
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Nickel-based layered hydroxides (LHs) are a family of efficientelectrocatalysts for the alkaline oxygen evolution reaction (OER).Nevertheless, fundamental aspects such as the influence of thecrystalline structure and the role of lattice distortion of thecatalytic sites remain poorly understood and typically muddled.Herein, we carried out a comprehensive investigation on ɑ-LH, β-LHand layered double hydroxide (LDH) phases by means of structural,spectroscopical, in-silico and electrochemical studies, whichsuggest the key aspect exerted by Ni-vacancies in the ɑ-LHstructure. Density functional theory (DFT) calculations and X-rayabsorption spectroscopy (XAS) confirm that the presence ofNi-vacancies produces acute distortions of the electroactive Ni sites(reflected as the shortening of the Ni−O distances and changes inthe O−Ni−O angles), triggering the appearance of Ni localisedelectronic states on the Fermi level, reducing the Egap, andconsequently, increasing the reactivity of the electroactive sites inthe ɑ-LH structure. Furthermore, post-mortem Raman and XASmeasurements unveil its transformation into a highly reactiveoxyhydroxide-like phase that remains stable under ambient conditions.Hence, this work pinpoints the critical role of the crystallinestructure as well as the electronic properties of LH structures ontheir inherent electrochemical reactivity towards OER catalysis. Weenvision Ni-based ɑ-LH as a perfect platform for hosting trivalentcations, closing the gap toward the next generation of benchmarkefficient earth-abundant electrocatalystsp.
Fil: Sanchis Gual, Roger. Universidad de Valencia; España
Fil: Jaramillo Hernández, Camilo. Universidad de Valencia; España
Fil: Hunt, Diego. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Oficina de Coordinacion Administrativa Ciudad Universitaria. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia - Nodo Constituyentes | Comision Nacional de Energia Atomica. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia - Nodo Constituyentes.; Argentina
Fil: Seijas Da Silva, Álvaro. Universidad de Valencia; España
Fil: Mizrahi, Martin Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Marini, Carlo. No especifíca;
Fil: Oestreicher, Víctor Santiago Jesús. Universidad de Valencia; España. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Abellán, Gonzalo. Universidad de Valencia; España
Materia
HYDROXIDES
DFT+U
EPOXIDE ROUTE
OER
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/231468
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/231468
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered HydroxidesSanchis Gual, RogerJaramillo Hernández, CamiloHunt, DiegoSeijas Da Silva, ÁlvaroMizrahi, Martin DanielMarini, CarloOestreicher, Víctor Santiago JesúsAbellán, GonzaloHYDROXIDESDFT+UEPOXIDE ROUTEOERhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Nickel-based layered hydroxides (LHs) are a family of efficientelectrocatalysts for the alkaline oxygen evolution reaction (OER).Nevertheless, fundamental aspects such as the influence of thecrystalline structure and the role of lattice distortion of thecatalytic sites remain poorly understood and typically muddled.Herein, we carried out a comprehensive investigation on ɑ-LH, β-LHand layered double hydroxide (LDH) phases by means of structural,spectroscopical, in-silico and electrochemical studies, whichsuggest the key aspect exerted by Ni-vacancies in the ɑ-LHstructure. Density functional theory (DFT) calculations and X-rayabsorption spectroscopy (XAS) confirm that the presence ofNi-vacancies produces acute distortions of the electroactive Ni sites(reflected as the shortening of the Ni−O distances and changes inthe O−Ni−O angles), triggering the appearance of Ni localisedelectronic states on the Fermi level, reducing the Egap, andconsequently, increasing the reactivity of the electroactive sites inthe ɑ-LH structure. Furthermore, post-mortem Raman and XASmeasurements unveil its transformation into a highly reactiveoxyhydroxide-like phase that remains stable under ambient conditions.Hence, this work pinpoints the critical role of the crystallinestructure as well as the electronic properties of LH structures ontheir inherent electrochemical reactivity towards OER catalysis. Weenvision Ni-based ɑ-LH as a perfect platform for hosting trivalentcations, closing the gap toward the next generation of benchmarkefficient earth-abundant electrocatalystsp.Fil: Sanchis Gual, Roger. Universidad de Valencia; EspañaFil: Jaramillo Hernández, Camilo. Universidad de Valencia; EspañaFil: Hunt, Diego. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Oficina de Coordinacion Administrativa Ciudad Universitaria. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia - Nodo Constituyentes | Comision Nacional de Energia Atomica. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia - Nodo Constituyentes.; ArgentinaFil: Seijas Da Silva, Álvaro. Universidad de Valencia; EspañaFil: Mizrahi, Martin Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Marini, Carlo. No especifíca;Fil: Oestreicher, Víctor Santiago Jesús. Universidad de Valencia; España. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Abellán, Gonzalo. Universidad de Valencia; EspañaJohn Wiley & Sons2023-11info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/231468Sanchis Gual, Roger; Jaramillo Hernández, Camilo; Hunt, Diego; Seijas Da Silva, Álvaro; Mizrahi, Martin Daniel; et al.; Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides; John Wiley & Sons; Chemistry - A European Journal; 30; 5; 11-2023; 1-121521-3765CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1002/chem.202303146info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:47:56Zoai:ri.conicet.gov.ar:11336/231468instacron: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:34982025-09-29 10:47:56.593CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
title Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
spellingShingle Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
Sanchis Gual, Roger
HYDROXIDES
DFT+U
EPOXIDE ROUTE
OER
title_short Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
title_full Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
title_fullStr Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
title_full_unstemmed Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
title_sort Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides
dc.creator.none.fl_str_mv Sanchis Gual, Roger
Jaramillo Hernández, Camilo
Hunt, Diego
Seijas Da Silva, Álvaro
Mizrahi, Martin Daniel
Marini, Carlo
Oestreicher, Víctor Santiago Jesús
Abellán, Gonzalo
author Sanchis Gual, Roger
author_facet Sanchis Gual, Roger
Jaramillo Hernández, Camilo
Hunt, Diego
Seijas Da Silva, Álvaro
Mizrahi, Martin Daniel
Marini, Carlo
Oestreicher, Víctor Santiago Jesús
Abellán, Gonzalo
author_role author
author2 Jaramillo Hernández, Camilo
Hunt, Diego
Seijas Da Silva, Álvaro
Mizrahi, Martin Daniel
Marini, Carlo
Oestreicher, Víctor Santiago Jesús
Abellán, Gonzalo
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv HYDROXIDES
DFT+U
EPOXIDE ROUTE
OER
topic HYDROXIDES
DFT+U
EPOXIDE ROUTE
OER
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Nickel-based layered hydroxides (LHs) are a family of efficientelectrocatalysts for the alkaline oxygen evolution reaction (OER).Nevertheless, fundamental aspects such as the influence of thecrystalline structure and the role of lattice distortion of thecatalytic sites remain poorly understood and typically muddled.Herein, we carried out a comprehensive investigation on ɑ-LH, β-LHand layered double hydroxide (LDH) phases by means of structural,spectroscopical, in-silico and electrochemical studies, whichsuggest the key aspect exerted by Ni-vacancies in the ɑ-LHstructure. Density functional theory (DFT) calculations and X-rayabsorption spectroscopy (XAS) confirm that the presence ofNi-vacancies produces acute distortions of the electroactive Ni sites(reflected as the shortening of the Ni−O distances and changes inthe O−Ni−O angles), triggering the appearance of Ni localisedelectronic states on the Fermi level, reducing the Egap, andconsequently, increasing the reactivity of the electroactive sites inthe ɑ-LH structure. Furthermore, post-mortem Raman and XASmeasurements unveil its transformation into a highly reactiveoxyhydroxide-like phase that remains stable under ambient conditions.Hence, this work pinpoints the critical role of the crystallinestructure as well as the electronic properties of LH structures ontheir inherent electrochemical reactivity towards OER catalysis. Weenvision Ni-based ɑ-LH as a perfect platform for hosting trivalentcations, closing the gap toward the next generation of benchmarkefficient earth-abundant electrocatalystsp.
Fil: Sanchis Gual, Roger. Universidad de Valencia; España
Fil: Jaramillo Hernández, Camilo. Universidad de Valencia; España
Fil: Hunt, Diego. Consejo Nacional de Investigaciones Cientificas y Tecnicas. Oficina de Coordinacion Administrativa Ciudad Universitaria. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia - Nodo Constituyentes | Comision Nacional de Energia Atomica. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia. Unidad Ejecutora Instituto de Nanociencia y Nanotecnologia - Nodo Constituyentes.; Argentina
Fil: Seijas Da Silva, Álvaro. Universidad de Valencia; España
Fil: Mizrahi, Martin Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Marini, Carlo. No especifíca;
Fil: Oestreicher, Víctor Santiago Jesús. Universidad de Valencia; España. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Abellán, Gonzalo. Universidad de Valencia; España
description Nickel-based layered hydroxides (LHs) are a family of efficientelectrocatalysts for the alkaline oxygen evolution reaction (OER).Nevertheless, fundamental aspects such as the influence of thecrystalline structure and the role of lattice distortion of thecatalytic sites remain poorly understood and typically muddled.Herein, we carried out a comprehensive investigation on ɑ-LH, β-LHand layered double hydroxide (LDH) phases by means of structural,spectroscopical, in-silico and electrochemical studies, whichsuggest the key aspect exerted by Ni-vacancies in the ɑ-LHstructure. Density functional theory (DFT) calculations and X-rayabsorption spectroscopy (XAS) confirm that the presence ofNi-vacancies produces acute distortions of the electroactive Ni sites(reflected as the shortening of the Ni−O distances and changes inthe O−Ni−O angles), triggering the appearance of Ni localisedelectronic states on the Fermi level, reducing the Egap, andconsequently, increasing the reactivity of the electroactive sites inthe ɑ-LH structure. Furthermore, post-mortem Raman and XASmeasurements unveil its transformation into a highly reactiveoxyhydroxide-like phase that remains stable under ambient conditions.Hence, this work pinpoints the critical role of the crystallinestructure as well as the electronic properties of LH structures ontheir inherent electrochemical reactivity towards OER catalysis. Weenvision Ni-based ɑ-LH as a perfect platform for hosting trivalentcations, closing the gap toward the next generation of benchmarkefficient earth-abundant electrocatalystsp.
publishDate 2023
dc.date.none.fl_str_mv 2023-11
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/11336/231468
Sanchis Gual, Roger; Jaramillo Hernández, Camilo; Hunt, Diego; Seijas Da Silva, Álvaro; Mizrahi, Martin Daniel; et al.; Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides; John Wiley & Sons; Chemistry - A European Journal; 30; 5; 11-2023; 1-12
1521-3765
CONICET Digital
CONICET
url http://hdl.handle.net/11336/231468
identifier_str_mv Sanchis Gual, Roger; Jaramillo Hernández, Camilo; Hunt, Diego; Seijas Da Silva, Álvaro; Mizrahi, Martin Daniel; et al.; Influence of Crystallographic Structure and Metal Vacancies on the Oxygen Evolution Reaction Performance of Ni-based Layered Hydroxides; John Wiley & Sons; Chemistry - A European Journal; 30; 5; 11-2023; 1-12
1521-3765
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1002/chem.202303146
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv John Wiley & Sons
publisher.none.fl_str_mv John Wiley & Sons
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 13.070432

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