Electrocatalytic CO2 Reduction with a Binuclear Bis-Terpyridine Pyrazole-Bridged Cobalt Complex
A pyrazole-based ligand substituted with terpyridine groups at the 3 and 5 positions has been synthesized to form the dinuclear cobalt complex 1, that electrocatalytically reduces carbon dioxide (CO2) to carbon monoxide (CO) in the presence of Bronsted acids in DMF. Chemical, electrochemical and UV-...
| Autores: | , , , , |
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| Tipo de recurso: | artículo |
| Estado: | Versión publicada |
| Fecha de publicación: | 2023 |
| País: | España |
| Institución: | Universidad de Sevilla (US) |
| Repositorio: | idUS. Depósito de Investigación de la Universidad de Sevilla |
| OAI Identifier: | oai:idus.us.es:11441/157356 |
| Acceso en línea: | https://hdl.handle.net/11441/157356 https://doi.org/10.1002/chem.202202361 |
| Access Level: | acceso abierto |
| Palabra clave: | Bimetallic Carbon dioxide Cobalt Electrocatalysis Spectro-electrochemistry |
| Sumario: | A pyrazole-based ligand substituted with terpyridine groups at the 3 and 5 positions has been synthesized to form the dinuclear cobalt complex 1, that electrocatalytically reduces carbon dioxide (CO2) to carbon monoxide (CO) in the presence of Bronsted acids in DMF. Chemical, electrochemical and UV-vis spectro-electrochemical studies under inert atmosphere indicate pairwise reduction processes of complex 1. Infrared spectro-electrochemical studies under CO2 and CO atmosphere are consistent with a reduced CO-containing dicobalt complex which results from the electroreduction of CO2. In the presence of trifluoroethanol (TFE), electrocatalytic studies revealed single-site mechanism with up to 94 % selectivity towards CO formation when 1.47 M TFE were present, at -1.35 V vs. Saturated Calomel Electrode in DMF (0.39 V overpotential). The low faradaic efficiencies obtained (<50 %) are attributed to the generation of CO-containing species formed during the electrocatalytic process, which inhibit the reduction of CO2. |
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