Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin

The electrochemical reduction of biomass-derived feedstocks provides a sustainable platform for the synthesis of a wide range of chemical commodities and biofuels. Despite their interest, the optimization of reaction conditions, the screening of electrode materials, and the mechanistic understanding...

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Autores: Gong, Li, Zhang, Chao Yue, Mu, Xiao, Han, Xu|||0000-0001-8319-8830, Li, Junshan|||0000-0002-1482-1972, Arbiol i Cobos, Jordi|||0000-0002-0695-1726, Zhou, Jin Yuan, Kallio, Tanja|||0000-0001-6671-8582, Martínez-Alanis, Paulina R.|||0000-0003-3675-4472, Cabot i Codina, Andreu|||0000-0002-7533-3251
Tipo de recurso: artículo
Fecha de publicación:2024
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:302106
Acceso en línea:https://ddd.uab.cat/record/302106
https://dx.doi.org/urn:doi:10.1016/j.cej.2023.147612
Access Level:acceso abierto
Palabra clave:Electrochemical reduction
Self-coupling
Semiconductor materials
Benzaldehyde
Hydrobenzoin
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spelling Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoinGong, LiZhang, Chao YueMu, XiaoHan, Xu|||0000-0001-8319-8830Li, Junshan|||0000-0002-1482-1972Arbiol i Cobos, Jordi|||0000-0002-0695-1726Zhou, Jin YuanKallio, Tanja|||0000-0001-6671-8582Martínez-Alanis, Paulina R.|||0000-0003-3675-4472Cabot i Codina, Andreu|||0000-0002-7533-3251Electrochemical reductionSelf-couplingSemiconductor materialsBenzaldehydeHydrobenzoinThe electrochemical reduction of biomass-derived feedstocks provides a sustainable platform for the synthesis of a wide range of chemical commodities and biofuels. Despite their interest, the optimization of reaction conditions, the screening of electrode materials, and the mechanistic understanding of these processes lag well behind other chemical routes. Here, we focus on the electrochemical self-coupling of benzaldehyde (BZH) to hydrobenzoin (HDB) using semiconductor electrocatalysts with nanosheet morphologies. By testing several semiconductor materials, a correlation is observed between their band gap and the electrochemical potential necessary to maximize selectivity towards HDB in alkaline medium, which we associate with the charge accumulation at the semiconductor surface. N-type CuInS provides the highest conversion rate at 0.3 mmol cmh with a selectivity of 98.5 % at -1.3 V vs. Hg/HgO. Additional density functional theory calculations demonstrate a lower kinetic energy barrier at the CuInS surface compared with graphitic carbon, proving its catalytic role in the self-coupling reaction of BZH. 22024-01-0120242024-01-01Articlehttp://purl.org/coar/resource_type/c_6501SMURhttp://purl.org/coar/version/c_71e4c1898caa6e32info:eu-repo/semantics/articleapplication/pdfhttps://ddd.uab.cat/record/302106https://dx.doi.org/urn:doi:10.1016/j.cej.2023.147612reponame:Dipòsit Digital de Documents de la UABinstname:Universitat Autònoma de BarcelonaInglésengEuropean Commission https://doi.org/10.13039/501100000780 801342Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2021/SGR-00457Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 CEX2021-001214-Sopen accesshttp://purl.org/coar/access_right/c_abf2Aquest material està protegit per drets d'autor i/o drets afins. Podeu utilitzar aquest material en funció del que permet la legislació de drets d'autor i drets afins d'aplicació al vostre cas. Per a d'altres usos heu d'obtenir permís del(s) titular(s) de drets.https://rightsstatements.org/vocab/InC/1.0/info:eu-repo/semantics/openAccessoai:ddd.uab.cat:3021062026-06-06T12:50:31Z
dc.title.none.fl_str_mv Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
title Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
spellingShingle Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
Gong, Li
Electrochemical reduction
Self-coupling
Semiconductor materials
Benzaldehyde
Hydrobenzoin
title_short Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
title_full Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
title_fullStr Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
title_full_unstemmed Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
title_sort Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin
dc.creator.none.fl_str_mv Gong, Li
Zhang, Chao Yue
Mu, Xiao
Han, Xu|||0000-0001-8319-8830
Li, Junshan|||0000-0002-1482-1972
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Zhou, Jin Yuan
Kallio, Tanja|||0000-0001-6671-8582
Martínez-Alanis, Paulina R.|||0000-0003-3675-4472
Cabot i Codina, Andreu|||0000-0002-7533-3251
author Gong, Li
author_facet Gong, Li
Zhang, Chao Yue
Mu, Xiao
Han, Xu|||0000-0001-8319-8830
Li, Junshan|||0000-0002-1482-1972
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Zhou, Jin Yuan
Kallio, Tanja|||0000-0001-6671-8582
Martínez-Alanis, Paulina R.|||0000-0003-3675-4472
Cabot i Codina, Andreu|||0000-0002-7533-3251
author_role author
author2 Zhang, Chao Yue
Mu, Xiao
Han, Xu|||0000-0001-8319-8830
Li, Junshan|||0000-0002-1482-1972
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Zhou, Jin Yuan
Kallio, Tanja|||0000-0001-6671-8582
Martínez-Alanis, Paulina R.|||0000-0003-3675-4472
Cabot i Codina, Andreu|||0000-0002-7533-3251
author2_role author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Electrochemical reduction
Self-coupling
Semiconductor materials
Benzaldehyde
Hydrobenzoin
topic Electrochemical reduction
Self-coupling
Semiconductor materials
Benzaldehyde
Hydrobenzoin
description The electrochemical reduction of biomass-derived feedstocks provides a sustainable platform for the synthesis of a wide range of chemical commodities and biofuels. Despite their interest, the optimization of reaction conditions, the screening of electrode materials, and the mechanistic understanding of these processes lag well behind other chemical routes. Here, we focus on the electrochemical self-coupling of benzaldehyde (BZH) to hydrobenzoin (HDB) using semiconductor electrocatalysts with nanosheet morphologies. By testing several semiconductor materials, a correlation is observed between their band gap and the electrochemical potential necessary to maximize selectivity towards HDB in alkaline medium, which we associate with the charge accumulation at the semiconductor surface. N-type CuInS provides the highest conversion rate at 0.3 mmol cmh with a selectivity of 98.5 % at -1.3 V vs. Hg/HgO. Additional density functional theory calculations demonstrate a lower kinetic energy barrier at the CuInS surface compared with graphitic carbon, proving its catalytic role in the self-coupling reaction of BZH.
publishDate 2024
dc.date.none.fl_str_mv 2
2024-01-01
2024
2024-01-01
dc.type.none.fl_str_mv Article
http://purl.org/coar/resource_type/c_6501
SMUR
http://purl.org/coar/version/c_71e4c1898caa6e32
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://ddd.uab.cat/record/302106
https://dx.doi.org/urn:doi:10.1016/j.cej.2023.147612
url https://ddd.uab.cat/record/302106
https://dx.doi.org/urn:doi:10.1016/j.cej.2023.147612
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 801342
Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2021/SGR-00457
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43
Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 CEX2021-001214-S
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://rightsstatements.org/vocab/InC/1.0/
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://rightsstatements.org/vocab/InC/1.0/
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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