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...
| Autores: | ; ; ; ; ; ; ; ; ; |
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| Tipo de documento: | Artículo |
| Fecha de publicación: | 2024 |
| País: | España |
| Institución: | Universitat Autònoma de Barcelona |
| Repositorio: | Dipòsit Digital de Documents de la UAB |
| Lenguaje: | 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 |
| Nivel de acceso: | Acceso abierto |
| Palabra clave: | Electrochemical reduction Self-coupling Semiconductor materials Benzaldehyde Hydrobenzoin |
| _version_ | 1878740489367191553 |
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| author | Gong, Li |
| 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 |
| author_browse | Arbiol i Cobos, Jordi|||0000-0002-0695-1726 Cabot i Codina, Andreu|||0000-0002-7533-3251 Gong, Li Han, Xu|||0000-0001-8319-8830 Kallio, Tanja|||0000-0001-6671-8582 Li, Junshan|||0000-0002-1482-1972 Martínez-Alanis, Paulina R.|||0000-0003-3675-4472 Mu, Xiao Zhang, Chao Yue Zhou, Jin Yuan |
| 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 |
| collection | Dipòsit Digital de Documents de la UAB |
| 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. |
| eu_rights_str_mv | openAccess |
| format | article |
| id | ES_d3fdfd591a9e5588b1afb1d3ddde35aa |
| institution | Universitat Autònoma de Barcelona |
| instname_str | Universitat Autònoma de Barcelona |
| language | eng |
| network_acronym_str | ES |
| network_name_str | España |
| oai_identifier_str | oai:ddd.uab.cat:302106 |
| publishDate | 2024 |
| publishDateSort | 2024 |
| reponame_str | Dipòsit Digital de Documents de la UAB |
| spelling | Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin 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 Electrochemical reduction Self-coupling Semiconductor materials Benzaldehyde 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 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. https://ddd.uab.cat/record/302106 https://dx.doi.org/urn:doi:10.1016/j.cej.2023.147612 |
| spellingShingle | Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin Gong, Li Electrochemical reduction Self-coupling Semiconductor materials Benzaldehyde Hydrobenzoin |
| title | 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_short | Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin |
| title_sort | Semiconductor nanosheets for electrocatalytic self-coupling of benzaldehyde to hydrobenzoin |
| topic | Electrochemical reduction Self-coupling Semiconductor materials Benzaldehyde Hydrobenzoin |
| topic_facet | Electrochemical reduction Self-coupling Semiconductor materials Benzaldehyde Hydrobenzoin |
| url | https://ddd.uab.cat/record/302106 https://dx.doi.org/urn:doi:10.1016/j.cej.2023.147612 |