Molecular engineering to introduce carbonyl between nickel salophen active sites to enhance electrochemical CO2 reduction to methanol

The electrochemical reduction of CO to methanol is a potentially cost-effective strategy to reduce the concentration of this greenhouse gas while at the same time producing a value-added chemical. Herein, we detail a highly efficient 2D nickel organic framework containing a large density of highly d...

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Detalles Bibliográficos
Autores: Liang, Zhifu, Wang, Jianghao, Tang, PengYi|||0000-0002-2306-095X, Tang, Weiqiang|||0000-0002-7726-4130, Liu, Lijia, Shakouri, Mohsen, Wang, Xiang, Llorca, Jordi|||0000-0002-7447-9582, Zhao, Shuangliang, Heggen, Marc|||0000-0002-2646-0078, Dunin-Borkowski, Rafal E.|||0000-0001-8082-0647, Cabot i Codina, Andreu|||0000-0002-7533-3251, Wu, Hao Bin, 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:266334
Acceso en línea:https://ddd.uab.cat/record/266334
https://dx.doi.org/urn:doi:10.1016/j.apcatb.2022.121451
Access Level:acceso abierto
Palabra clave:Two dimensional π-d organic frameworks
Atomically dispersed nickel
Carbonyl group
Electrocatalytic CO2 reduction
Methanol
Descripción
Sumario:The electrochemical reduction of CO to methanol is a potentially cost-effective strategy to reduce the concentration of this greenhouse gas while at the same time producing a value-added chemical. Herein, we detail a highly efficient 2D nickel organic framework containing a large density of highly dispersed salophen NiNO active sites toward electrochemical CORR to methanol. By tuning the ligand environment of the salophen NiNO, the electrocatalytic activity of the material toward CO reduction can be significantly improved. We prove that by introducing a carbonyl group at the ligand environment of the Ni active sites, the electrochemical CO reduction activity is highly promoted and its product selectivity reaches a Faradaic efficiency of 27% toward the production of methanol at - 0.9 V vs RHE. The salophen-based π-d conjugated metal-organic framework presented here thus provides the best performance toward CO reduction to methanol among the previously developed nickel-based electrocatalysts.