An Iron Pyridyl-Carbene Electrocatalyst for Low Overpotential CO2 Reduction to CO
Electrocatalysts for CO2 reduction based on first row transition metal ions have attracted attention as abundant and affordable candidates for energy conversion applications. Yet, very few molecular iron electrocatalysts exhibit high selectivity for CO. Iron complexes supported by a redox-active 2,2...
| Autores: | , , |
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| Tipo de recurso: | artículo |
| Estado: | Versión aceptada para publicación |
| Fecha de publicación: | 2020 |
| País: | España |
| Institución: | Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya) |
| Repositorio: | Recercat. Dipósit de la Recerca de Catalunya |
| OAI Identifier: | oai:recercat.cat:2072/443470 |
| Acceso en línea: | http://hdl.handle.net/2072/443470 https://doi.org/10.1021/acscatal.0c03798 |
| Access Level: | acceso abierto |
| Palabra clave: | 54 |
| Sumario: | Electrocatalysts for CO2 reduction based on first row transition metal ions have attracted attention as abundant and affordable candidates for energy conversion applications. Yet, very few molecular iron electrocatalysts exhibit high selectivity for CO. Iron complexes supported by a redox-active 2,2':6',2''-terpyridine (tpy) ligand and a strong trans effect pyridyl-N-heterocyclic carbene ligand (1-methyl-benzimidazol-2-ylidene-3-(2-pyridine)) were synthesized and found to catalyze the selective electroreduction of CO2 to CO at very low overpotential. Mechanistic studies using electrochemical and computational methods provided insight into the nature of catalytic intermediates that guided the development of continuous CO2 flow conditions that improved performance, producing CO with >95% Faradaic efficiency at only 150 mV overpotential. The studies reveal general design principles for non-heme iron electrocatalysts, including the importance of lability and geometric isomerization, that can serve to guide future developments in the design of affordable and efficient catalysts for CO2 electroreduction. |
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