Steering the Reaction Pathway of CO 2 Electroreduction by Tuning the Coordination Number of Copper Catalysts

• Published in: Journal of the American Chemical Society 2024-06, Vol.146 (23), p.15917
• Main Authors: Jiao, Jiapeng, Kang, Xinchen, Yang, Jiahao, Jia, Shuaiqiang, Peng, Yaguang, Liu, Shiqiang, Chen, Chunjun, Xing, Xueqing, He, Mingyuan, Wu, Haihong, Han, Buxing
• Format: Article
• Language: English
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.4c02607

Cu-based catalysts are optimal for the electroreduction of CO to generate hydrocarbon products. However, controlling product distribution remains a challenging topic. The theoretical investigations have revealed that the coordination number (CN) of Cu considerably influences the adsorption energy of *CO intermediates, thereby affecting the reaction pathway. Cu catalysts with different CNs were fabricated by reducing CuO precursors via cyclic voltammetry (Cyc-Cu), potentiostatic electrolysis (Pot-Cu), and pulsed electrolysis (Pul-Cu), respectively. High-CN Cu catalysts predominantly generate C products, while low-CN Cu favors CH production. For instance, over the high-CN Pot-Cu, C is the main product, with the Faradaic efficiency (FE) reaching 82.5% and a partial current density ( ) of 514.3 mA cm . Conversely, the low-CN Pul(3)-Cu favors the production of CH , achieving the highest FE value of 56.7% with a value of 234.4 mA cm . In situ X-ray absorption spectroscopy and Raman spectroscopy studies further confirm the different *CO adsorptions over Cu catalysts with different CN, thereby directing the reaction pathway of the CO RR.