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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| Format: | Article |
| Publication date: | 2024 |
| Country: | España |
| Institution: | Universitat Autònoma de Barcelona |
| Repository: | Dipòsit Digital de Documents de la UAB |
| Language: | English |
| OAI Identifier: | oai:ddd.uab.cat:302106 |
| Online Access: | https://ddd.uab.cat/record/302106 https://dx.doi.org/urn:doi:10.1016/j.cej.2023.147612 |
| Access Level: | Open access |
| Keyword: | Electrochemical reduction Self-coupling Semiconductor materials Benzaldehyde Hydrobenzoin |
| Summary: | 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. |
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