Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation

Atomically dispersed metals maximize the number of catalytic sites and enhance their activity. However, their challenging synthesis and characterization strongly complicates their optimization. Here, the aim is to demonstrate that tuning the electronic environment of atomically dispersed metal catal...

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Autores: Liang, Zhifu, Jiang, Daochuan, Wang, Xiang, Shakouri, Mohsen, Zhang, Ting|||0000-0002-0317-9662, Li, Zhongjun, Tang, PengYi|||0000-0002-2306-095X, Llorca, Jordi|||0000-0002-7447-9582, Liu, Lijia, Yuan, Yupeng, Heggen, Marc|||0000-0002-2646-0078, Dunin-Borkowski, Rafal E.|||0000-0001-8082-0647, Morante, Joan Ramon|||0000-0002-4981-4633, Cabot i Codina, Andreu|||0000-0002-7533-3251, Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Tipo de recurso: artículo
Fecha de publicación:2021
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:268423
Acceso en línea:https://ddd.uab.cat/record/268423
https://dx.doi.org/urn:doi:10.1002/adfm.202106349
Access Level:acceso abierto
Palabra clave:Alcohol oxidation
Atomically dispersed metals
Electrocatalytic oxidation
Nickel
2D organic frameworks
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spelling Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidationLiang, ZhifuJiang, DaochuanWang, XiangShakouri, MohsenZhang, Ting|||0000-0002-0317-9662Li, ZhongjunTang, PengYi|||0000-0002-2306-095XLlorca, Jordi|||0000-0002-7447-9582Liu, LijiaYuan, YupengHeggen, Marc|||0000-0002-2646-0078Dunin-Borkowski, Rafal E.|||0000-0001-8082-0647Morante, Joan Ramon|||0000-0002-4981-4633Cabot i Codina, Andreu|||0000-0002-7533-3251Arbiol i Cobos, Jordi|||0000-0002-0695-1726Alcohol oxidationAtomically dispersed metalsElectrocatalytic oxidationNickel2D organic frameworksAtomically dispersed metals maximize the number of catalytic sites and enhance their activity. However, their challenging synthesis and characterization strongly complicates their optimization. Here, the aim is to demonstrate that tuning the electronic environment of atomically dispersed metal catalysts through the modification of their edge coordination is an effective strategy to maximize their performance. This article focuses on optimizing nickel-based electrocatalysts toward alcohol electrooxidation in alkaline solution. A new organic framework with atomically dispersed nickel is first developed. The coordination environment of nickel within this framework is modified through the addition of carbonyl (CO) groups. The authors then demonstrate that such nickel-based organic frameworks, combined with carbon nanotubes, exhibit outstanding catalytic activity and durability toward the oxidation of methanol (CHOH), ethanol (CHCHOH), and benzyl alcohol (CHCHOH); the smaller molecule exhibits higher catalytic performance. These outstanding electrocatalytic activities for alcohol electrooxidation are attributed to the presence of the carbonyl group in the ligand chemical environment, which enhances the adsorption for alcohol, as revealed by density functional theory calculations. The work not only introduces a new atomically dispersed Ni-based catalyst, but also demonstrates a new strategy for designing and engineering high-performance catalysts through the tuning of their chemical environment. 22021-01-0120212021-01-01Articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://ddd.uab.cat/record/268423https://dx.doi.org/urn:doi:10.1002/adfm.202106349reponame:Dipòsit Digital de Documents de la UABinstname:Universitat Autònoma de BarcelonaInglésengEuropean Commission https://doi.org/10.13039/501100000780 823717Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 RTI2018-093996-B-C31Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 SEV-2017-0706Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 ENE2017-85087-C3Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 ENE2016-77798-C4-3-RMinisterio de Economía y Competitividad https://doi.org/10.13039/501100003329 SEV-2013-0295-17-1Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-1246Agència 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-128open 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, i la comunicació pública de l'obra, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original. No es permet la creació d'obres derivades.https://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:ddd.uab.cat:2684232026-06-06T12:50:31Z
dc.title.none.fl_str_mv Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
title Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
spellingShingle Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
Liang, Zhifu
Alcohol oxidation
Atomically dispersed metals
Electrocatalytic oxidation
Nickel
2D organic frameworks
title_short Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
title_full Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
title_fullStr Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
title_full_unstemmed Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
title_sort Molecular engineering to tune the ligand environment of atomically dispersed nickel for efficient alcohol electrochemical oxidation
dc.creator.none.fl_str_mv Liang, Zhifu
Jiang, Daochuan
Wang, Xiang
Shakouri, Mohsen
Zhang, Ting|||0000-0002-0317-9662
Li, Zhongjun
Tang, PengYi|||0000-0002-2306-095X
Llorca, Jordi|||0000-0002-7447-9582
Liu, Lijia
Yuan, Yupeng
Heggen, Marc|||0000-0002-2646-0078
Dunin-Borkowski, Rafal E.|||0000-0001-8082-0647
Morante, Joan Ramon|||0000-0002-4981-4633
Cabot i Codina, Andreu|||0000-0002-7533-3251
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
author Liang, Zhifu
author_facet Liang, Zhifu
Jiang, Daochuan
Wang, Xiang
Shakouri, Mohsen
Zhang, Ting|||0000-0002-0317-9662
Li, Zhongjun
Tang, PengYi|||0000-0002-2306-095X
Llorca, Jordi|||0000-0002-7447-9582
Liu, Lijia
Yuan, Yupeng
Heggen, Marc|||0000-0002-2646-0078
Dunin-Borkowski, Rafal E.|||0000-0001-8082-0647
Morante, Joan Ramon|||0000-0002-4981-4633
Cabot i Codina, Andreu|||0000-0002-7533-3251
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
author_role author
author2 Jiang, Daochuan
Wang, Xiang
Shakouri, Mohsen
Zhang, Ting|||0000-0002-0317-9662
Li, Zhongjun
Tang, PengYi|||0000-0002-2306-095X
Llorca, Jordi|||0000-0002-7447-9582
Liu, Lijia
Yuan, Yupeng
Heggen, Marc|||0000-0002-2646-0078
Dunin-Borkowski, Rafal E.|||0000-0001-8082-0647
Morante, Joan Ramon|||0000-0002-4981-4633
Cabot i Codina, Andreu|||0000-0002-7533-3251
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Alcohol oxidation
Atomically dispersed metals
Electrocatalytic oxidation
Nickel
2D organic frameworks
topic Alcohol oxidation
Atomically dispersed metals
Electrocatalytic oxidation
Nickel
2D organic frameworks
description Atomically dispersed metals maximize the number of catalytic sites and enhance their activity. However, their challenging synthesis and characterization strongly complicates their optimization. Here, the aim is to demonstrate that tuning the electronic environment of atomically dispersed metal catalysts through the modification of their edge coordination is an effective strategy to maximize their performance. This article focuses on optimizing nickel-based electrocatalysts toward alcohol electrooxidation in alkaline solution. A new organic framework with atomically dispersed nickel is first developed. The coordination environment of nickel within this framework is modified through the addition of carbonyl (CO) groups. The authors then demonstrate that such nickel-based organic frameworks, combined with carbon nanotubes, exhibit outstanding catalytic activity and durability toward the oxidation of methanol (CHOH), ethanol (CHCHOH), and benzyl alcohol (CHCHOH); the smaller molecule exhibits higher catalytic performance. These outstanding electrocatalytic activities for alcohol electrooxidation are attributed to the presence of the carbonyl group in the ligand chemical environment, which enhances the adsorption for alcohol, as revealed by density functional theory calculations. The work not only introduces a new atomically dispersed Ni-based catalyst, but also demonstrates a new strategy for designing and engineering high-performance catalysts through the tuning of their chemical environment.
publishDate 2021
dc.date.none.fl_str_mv 2
2021-01-01
2021
2021-01-01
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/268423
https://dx.doi.org/urn:doi:10.1002/adfm.202106349
url https://ddd.uab.cat/record/268423
https://dx.doi.org/urn:doi:10.1002/adfm.202106349
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv European Commission https://doi.org/10.13039/501100000780 823717
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 RTI2018-093996-B-C31
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43
Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 SEV-2017-0706
Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 ENE2017-85087-C3
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 ENE2016-77798-C4-3-R
Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 SEV-2013-0295-17-1
Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-1246
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-128
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://creativecommons.org/licenses/by-nc-nd/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-nc-nd/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
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repository.mail.fl_str_mv
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