Enhanced CO Affinity on Cu Facilitates CO2 Electroreduction toward Multi‐Carbon Products

• Published in: Small (Weinheim an der Bergstrasse, Germany) Germany), 2023-09, Vol.19 (39), p.e2302530-e2302530
• Main Authors: Li, Xiaotong, Qin, Minkai, Wu, Xiuju, Lv, Xiangzhou, Wang, Jianghao, Wang, Yong, Hao Bin Wu
• Format: Article
• Language: English
• Subjects: Affinity; Bimetals; Carbon dioxide; Carbon monoxide; Catalysts; Chemical reduction; Current density; Density functional theory; Electric energy storage; Frequencies; Gibbs free energy; Nanotechnology; Palladium; Raman spectra
• ISSN: 1613-6810; 1613-6829
• DOI: 10.1002/smll.202302530

Electrochemical CO2 reduction reaction (CO2RR) is a promising strategy for waste CO2 utilization and intermittent electricity storage. Herein, it is reported that bimetallic Cu/Pd catalysts with enhanced *CO affinity show a promoted CO2RR performance for multi‐carbon (C2+) production under industry‐relevant high current density. Especially, bimetallic Cu/Pd‐1% catalyst shows an outstanding CO2‐to‐C2+ conversion with 66.2% in Faradaic efficiency (FE) and 463.2 mA cm−2 in partial current density. An increment in the FE ratios of C2+ products to CO for Cu/Pd‐1% catalyst further illuminates a preferable C2+ production. In situ Raman spectra reveal that the atop‐bounded CO is dominated by low‐frequency band CO on Cu/Pd‐1% that leads to C2+ products on bimetallic catalysts, in contrast to the majority of high‐frequency band CO on Cu that favors the formation of CO. Density function theory calculation confirms that bimetallic Cu/Pd catalyst enhances the *CO adsorption and reduces the Gibbs free energy of the CC coupling process, thereby favoring the formation of C2+ products.