Lewis Acidic Support Boosts C-C Coupling in the Pulsed Electrochemical CO2 Reaction.
J Am Chem Soc
; 145(12): 6953-6965, 2023 Mar 29.
Article
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| MEDLINE
| ID: mdl-36921031
ABSTRACT
Copper-oxide electrocatalysts have been demonstrated to effectively perform the electrochemical CO2 reduction reaction (CO2RR) toward C2+ products, yet preserving the reactive high-valent CuOx has remained elusive. Herein, we demonstrate a model system of Lewis acidic supported Cu electrocatalyst with a pulsed electroreduction method to achieve enhanced performance for C2+ products, in which an optimized electrocatalyst could reach â¼76% Faradaic efficiency for C2+ products (FEC2+) at â¼-0.99 V versus reversible hydrogen electrode, and the corresponding mass activity can be enhanced by â¼2 times as compared to that of conventional CuOx. In situ time-resolved X-ray absorption spectroscopy investigating the dynamic chemical/physical nature of Cu during CO2RR discloses that an activation process induced by the KOH electrolyte during pulsed electroreduction greatly enriched the Cuδ+O/Znδ+O interfaces, which further reveals that the presence of Znδ+O species under the cathodic potential could effectively serve as a Lewis acidic support for preserving the Cuδ+O species to facilitate the formation of C2+ products, and the catalyst structure-property relationship of Cuδ+O/Znδ+O interfaces can be evidently realized. More importantly, we find a universality of stabilizing Cuδ+O species for various metal oxide supports and to provide a general concept of appropriate electrocatalyst-Lewis acidic support interaction for promoting C2+ products.
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J Am Chem Soc
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2023
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Article