CuGa Alloy Catalysts Enable C–C Coupling for Electrocatalytic CO 2 Reduction into C 2+ Products

法拉第效率 催化作用 电催化剂 材料科学 电化学 吸附 选择性 密度泛函理论 电解 化学工程 合金 退火(玻璃) 无机化学 电流密度 纳米技术 氧化还原 多相催化 化学 储能 联轴节(管道) 碳纤维
作者
Tongxin Qu,Yongchun Zhao,Zhuo Xiong,Junying Zhang
出处
期刊:ACS applied energy materials [American Chemical Society]
卷期号:9 (3): 1466-1478
标识
DOI:10.1021/acsaem.5c03181
摘要

Electrocatalytic CO 2 reduction reaction (eCO 2 RR) offers a sustainable route for converting CO 2 into value-added chemicals, contributing to carbon neutrality. While high selectivity toward C 1 products has been achieved, the efficient production of multicarbon (C 2+ ) compounds remains challenging due to the high energy barriers of C–C coupling. Copper-based catalysts are promising for C 2+ generation owing to their unique *CO binding energy, yet they suffer from low selectivity and stability. Alloying copper (Cu) with other metals is an effective strategy for regulating intermediate adsorption and facilitating C–C coupling. In this study, an efficient CuGa solid solution alloy electrocatalyst for the eCO 2 RR was synthesized, employing only straightforward immersion drying and subsequent reduction annealing processes. At an applied potential of −1.19 V vs RHE, this catalyst exhibited a high Faradaic efficiency of 66.27% for C 2+ products, significantly suppressing C 1 pathways. It also demonstrated remarkable stability, maintaining structural and morphological integrity even after 12 h of electrolysis at a current density of 300 mA/cm 2 . Density functional theory calculation integrated with in situ characterization revealed that synergistic interaction between Cu and Ga enhances the adsorption of key intermediates (*COOH and *CO) and reduces the energy barrier of *CO dimerization. This work provides insights into the design of efficient and stable Cu-based electrocatalysts for C 2+ production via an electrochemical method.
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