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Pàgina inicial > Articles > Articles publicats > Metal oxide clusters on nitrogen-doped carbon are highly selective for CO2 electroreduction to CO |
Data: | 2021 |
Resum: | The electrochemical reduction of CO2 (eCO2RR) using renewable energy is an effective approach to pursue carbon neutrality. The eCO2RR to CO is indispensable in promoting C-C coupling through bifunctional catalysis and achieving cascade conversion from CO2 to C2+. This work investigates a series of M/N-C (M = Mn, Fe, Co, Ni, Cu, and Zn) catalysts, for which the metal precursor interacted with the nitrogen-doped carbon support (N-C) at room temperature, resulting in the metal being present as (sub)nanosized metal oxide clusters under ex situ conditions, except for Cu/N-C and Zn/N-C. A volcano trend in their activity toward CO as a function of the group of the transition metal is revealed, with Co/N-C exhibiting the highest activity at -0. 5 V versus RHE, while Ni/N-C shows both appreciable activity and selectivity. Operando X-ray absorption spectroscopy shows that the majority of Cu atoms in Cu/N-C form Cu0 clusters during eCO2RR, while Mn/, Fe/, Co/, and Ni/N-C catalysts maintain the metal hydroxide structures, with a minor amount of M0 formed in Fe/, Co/, and Ni/N-C. The superior activity of Fe/, Co/, and Ni/N-C is ascribed to the phase contraction and the HCO3- insertion into the layered structure of metal hydroxides. Our work provides a facile synthetic approach toward highly active and selective electrocatalysts to convert CO2 into CO. Coupled with state-of-the-art NiFe-based anodes in a full-cell device, Ni/N-C exhibits >80% Faradaic efficiency toward CO at 100 mA cm-2. |
Ajuts: | European Commission 732840 Ministerio de Economía y Competitividad CEX2019-000925-S Ministerio de Ciencia e Innovación RTI2018-095618-B-I00 Ministerio de Ciencia e Innovación ENE2017-85087-C3 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-1406 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-327 |
Drets: | Tots els drets reservats. |
Llengua: | Anglès |
Document: | Article ; recerca ; Versió sotmesa a revisió |
Matèria: | Catalysts ; Materials ; Metals ; Transition metals ; X-ray absorption near edge spectroscopy |
Publicat a: | ACS catalysis, Vol. 11, issue 15 (August 2021) , p. 10028-10042, ISSN 2155-5435 |
Preprint 43 p, 4.9 MB |