Lewis Acidic Support Boosts C-C Coupling in the Pulsed Electrochemical CO2 Reaction
Journal
Journal of the American Chemical Society
Journal Volume
145
Journal Issue
12
Pages
6953
Date Issued
2023-03-29
Author(s)
Chang, Chia-Jui
Lai, Yi-An
Chu, You-Chiuan
Peng, Chun-Kuo
Tan, Hui-Ying
Pao, Chih-Wen
Lin, Yan-Gu
Hung, Sung-Fu
Chen, Hsiao-Chien
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 ∼76% Faradaic efficiency for C2+ products (FEC2+) at ∼-0.99 V versus reversible hydrogen electrode, and the corresponding mass activity can be enhanced by ∼2 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.
Subjects
RAY-ABSORPTION SPECTROSCOPY; CARBON-DIOXIDE; COPPER-CATALYSTS; REDUCTION; CU2O; ELECTROREDUCTION; DESIGN; STATE
Publisher
AMER CHEMICAL SOC
Type
journal article