Copper‐Catalysed Electrochemical CO<sub>2</sub> Methanation via the Alloying of Single Cobalt Atoms
Jiawei Li, Miaojin Wei, Bifa Ji, Sunpei Hu, Jing Xue, Donghao Zhao, Haoyuan Wang, Chunxiao Liu, Yifan Ye, Jilong Xu, Jie Zeng, Ruquan Ye, Yongping Zheng, Tingting Zheng, Chuan Xia
Abstract
Abstract The electrochemical reduction of carbon dioxide (CO 2 ) to methane (CH 4 ) presents a promising solution for mitigating CO 2 emissions while producing valuable chemical feedstocks. Although single‐atom catalysts have shown potential in selectively converting CO 2 to CH 4 , their limited active sites often hinder the realization of high current densities, posing a selectivity‐activity dilemma. In this study, we developed a single‐atom cobalt (Co) doped copper catalyst (Co 1 Cu) that achieved a CH 4 Faradaic efficiency exceeding 60 % with a partial current density of −482.7 mA cm −2 . Mechanistic investigations revealed that the incorporation of single Co atoms enhances the activation and dissociation of H 2 O molecules, thereby lowering the energy barrier for the hydrogenation of *CO intermediates. In situ spectroscopic experiments and density functional theory simulations further demonstrated that the modulation of the *CO adsorption configuration, with stronger bridge‐binding, favours deep reduction to CH 4 over the C−C coupling or CO desorption pathways. Our findings underscore the potential of Co 1 Cu catalysts in overcoming the selectivity‐activity trade‐off, paving the way for efficient and scalable CO 2 ‐to‐CH 4 conversion technologies.