Stabilization of oxidized Cu species via CeO x nano-islands for enhanced CO2 reduction to C2+ products

作者：Miaojin Wei, Jiawei Li, Jiankang Zhao, Sunpei Hu, Yongsheng Ji, Weiqing Xue, Yizhou Dai, Haoyuan Wang, Xinyan Zhang, Kwun Nam Hui, Xu Li, Chuan Xia, Tingting Zheng, Jie Zeng · 发表于：National Science Review · 年份：2025 · DOI：10.1093/nsr/nwaf351 · 被引用次数：28 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Catalysts for Methane Reforming

ABSTRACT The presence of oxidized copper species (CuOx) on metallic Cu surfaces is widely acknowledged as a critical factor for promoting C–C coupling during the CO2 reduction reactions (CO2RR). However, the inherent instability of CuOx under negative potentials, where it is prone to reduction to metallic Cu, remains a formidable challenge. In this study, we developed a CeOx-modified CuO catalyst for the CO2RR, featuring CeOx uniformly distributed as isolated nano-islands on CuO nanoparticles. Upon reduction of the CuO matrix to metallic Cu, the CeOx layer effectively stabilizes the interfacial CuOx, preventing its further reduction. Operando characterization verified the sustained presence of Cu2+ and Cu+ species at highly reductive potentials, underscoring the role of CeOx in preserving CuOx stability. Theoretical calculations revealed that Ce3+ enhances the formation energy of oxygen vacancies, stabilizing the CuOx interface and *OC–CO intermediates, which are crucial for C–C coupling. With this surface modification strategy, the catalyst achieved a remarkable C2+ faradaic efficiency of 78% at −700 mA cm−2, while demonstrating persistent performance with a faradaic efficiency exceeding 70% for C2+ products at −100 mA cm−2 for over 110 h. These findings present an effective strategy for stabilizing metal oxides and advancing durable CO2RR catalysts.