Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction

The adsorption and activation of CO on the electrode interface is a prerequisite and key step for electrocatalytic CO reduction reaction (eCO RR). Regulating the interfacial microenvironment to promote the adsorption and activation of CO is thus of great significance to optimize overall conversion e...

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Autores: Han, Xu|||0000-0001-8319-8830, Zhang, Ting, Biset-Peiró, Martí|||0000-0002-1255-7733, Zhang, Xuan|||0000-0002-3667-4280, Li, Jian, Tang, Weiqiang|||0000-0002-7726-4130, Tang, PengYi|||0000-0002-2306-095X, Morante, Joan Ramon|||0000-0002-4981-4633, Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Tipo de recurso: artículo
Fecha de publicación:2022
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:264901
Acceso en línea:https://ddd.uab.cat/record/264901
https://dx.doi.org/urn:doi:10.1021/acsami.2c09129
Access Level:acceso abierto
Palabra clave:ZnO
Surficial hydroxyls
CO adsorption
CO activation
Metal-organic frameworks (MOFs)
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spelling Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO ReductionHan, Xu|||0000-0001-8319-8830Zhang, TingBiset-Peiró, Martí|||0000-0002-1255-7733Zhang, Xuan|||0000-0002-3667-4280Li, JianTang, Weiqiang|||0000-0002-7726-4130Tang, PengYi|||0000-0002-2306-095XMorante, Joan Ramon|||0000-0002-4981-4633Arbiol i Cobos, Jordi|||0000-0002-0695-1726ZnOSurficial hydroxylsCO adsorptionCO activationMetal-organic frameworks (MOFs)The adsorption and activation of CO on the electrode interface is a prerequisite and key step for electrocatalytic CO reduction reaction (eCO RR). Regulating the interfacial microenvironment to promote the adsorption and activation of CO is thus of great significance to optimize overall conversion efficiency. Herein, a CO-philic hydroxyl coordinated ZnO (ZnO-OH) catalyst is fabricated, for the first time, via a facile MOF-assisted method. In comparison to the commercial ZnO, the as-prepared ZnO-OH exhibits much higher selectivity toward CO at lower applied potential, reaching a Faradaic efficiency of 85% at -0.95 V versus RHE. To the best of our knowledge, such selectivity is one of the best records in ZnO-based catalysts reported till date. Density functional theory calculations reveal that the coordinated surficial -OH groups are not only favorable to interact with CO molecules but also function in synergy to decrease the energy barrier of the rate-determining step and maintain a higher charge density of potential active sites as well as inhibit undesired hydrogen evolution reaction. Our results indicate that engineering the interfacial microenvironment through the introduction of CO-philic groups is a promising way to achieve the global optimization of eCO RR via promoting adsorption and activation of CO. 22022-01-0120222022-01-01Articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://ddd.uab.cat/record/264901https://dx.doi.org/urn:doi:10.1021/acsami.2c09129reponame:Dipòsit Digital de Documents de la UABinstname:Universitat Autònoma de BarcelonaInglésengAgència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-327Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-1246Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C42Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 SEV-2017-0706open accesshttp://purl.org/coar/access_right/c_abf2Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.https://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:ddd.uab.cat:2649012026-06-06T12:50:31Z
dc.title.none.fl_str_mv Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
title Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
spellingShingle Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
Han, Xu|||0000-0001-8319-8830
ZnO
Surficial hydroxyls
CO adsorption
CO activation
Metal-organic frameworks (MOFs)
title_short Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
title_full Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
title_fullStr Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
title_full_unstemmed Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
title_sort Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction
dc.creator.none.fl_str_mv Han, Xu|||0000-0001-8319-8830
Zhang, Ting
Biset-Peiró, Martí|||0000-0002-1255-7733
Zhang, Xuan|||0000-0002-3667-4280
Li, Jian
Tang, Weiqiang|||0000-0002-7726-4130
Tang, PengYi|||0000-0002-2306-095X
Morante, Joan Ramon|||0000-0002-4981-4633
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
author Han, Xu|||0000-0001-8319-8830
author_facet Han, Xu|||0000-0001-8319-8830
Zhang, Ting
Biset-Peiró, Martí|||0000-0002-1255-7733
Zhang, Xuan|||0000-0002-3667-4280
Li, Jian
Tang, Weiqiang|||0000-0002-7726-4130
Tang, PengYi|||0000-0002-2306-095X
Morante, Joan Ramon|||0000-0002-4981-4633
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
author_role author
author2 Zhang, Ting
Biset-Peiró, Martí|||0000-0002-1255-7733
Zhang, Xuan|||0000-0002-3667-4280
Li, Jian
Tang, Weiqiang|||0000-0002-7726-4130
Tang, PengYi|||0000-0002-2306-095X
Morante, Joan Ramon|||0000-0002-4981-4633
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv ZnO
Surficial hydroxyls
CO adsorption
CO activation
Metal-organic frameworks (MOFs)
topic ZnO
Surficial hydroxyls
CO adsorption
CO activation
Metal-organic frameworks (MOFs)
description The adsorption and activation of CO on the electrode interface is a prerequisite and key step for electrocatalytic CO reduction reaction (eCO RR). Regulating the interfacial microenvironment to promote the adsorption and activation of CO is thus of great significance to optimize overall conversion efficiency. Herein, a CO-philic hydroxyl coordinated ZnO (ZnO-OH) catalyst is fabricated, for the first time, via a facile MOF-assisted method. In comparison to the commercial ZnO, the as-prepared ZnO-OH exhibits much higher selectivity toward CO at lower applied potential, reaching a Faradaic efficiency of 85% at -0.95 V versus RHE. To the best of our knowledge, such selectivity is one of the best records in ZnO-based catalysts reported till date. Density functional theory calculations reveal that the coordinated surficial -OH groups are not only favorable to interact with CO molecules but also function in synergy to decrease the energy barrier of the rate-determining step and maintain a higher charge density of potential active sites as well as inhibit undesired hydrogen evolution reaction. Our results indicate that engineering the interfacial microenvironment through the introduction of CO-philic groups is a promising way to achieve the global optimization of eCO RR via promoting adsorption and activation of CO.
publishDate 2022
dc.date.none.fl_str_mv 2
2022-01-01
2022
2022-01-01
dc.type.none.fl_str_mv Article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://ddd.uab.cat/record/264901
https://dx.doi.org/urn:doi:10.1021/acsami.2c09129
url https://ddd.uab.cat/record/264901
https://dx.doi.org/urn:doi:10.1021/acsami.2c09129
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-327
Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-1246
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C42
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43
Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 SEV-2017-0706
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:Dipòsit Digital de Documents de la UAB
instname:Universitat Autònoma de Barcelona
instname_str Universitat Autònoma de Barcelona
reponame_str Dipòsit Digital de Documents de la UAB
collection Dipòsit Digital de Documents de la UAB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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