Zhao Zhenwei, Zhang Yu, Li Junjun, Yao Bingqing, Zhang Hui, Zhang Zhicheng
Department of Chemistry, School of Science, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Tianjin University, Tianjin, 300072, China.
Center for Computational Chemistry and Molecular Simulation, College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu, 610500, China.
Angew Chem Int Ed Engl. 2025 Aug 25;64(35):e202510383. doi: 10.1002/anie.202510383. Epub 2025 Jul 16.
Rational design of water activation center to promote active hydrogen (*H) generation and stabilize Cu(I) species are significant for the formation of multicarbon (C) products over Cu-based catalysts in electrocatalytic CO reduction reaction (CORR). Herein, CeO nanograins and CuO nanothorns were selectively deposited on the edges of CuO cubes through the seed-mediated growth method. The as-synthesized CuO-CeO composites exhibit enhanced Faradaic efficiency and partial current density of CH compared with CuO cubes. In situ spectroscopies and theoretical calculations confirm that the Cu-O-Ce bridges in CuO-CeO composite can effectively enhance *H absorption and stabilize Cu(I) species, facilitating subsequent C-C coupling and further protonation into the key *COCHO intermediate of CH. This work provides new insights into modulating *H absorption and stabilizing Cu(I) species for boosting CO to C products.
合理设计水活化中心以促进活性氢（H）的产生并稳定Cu（I）物种，对于在电催化CO还原反应（CORR）中基于铜的催化剂上形成多碳（C）产物具有重要意义。在此，通过种子介导生长法将CeO纳米颗粒和CuO纳米刺选择性地沉积在CuO立方体的边缘。与CuO立方体相比，合成的CuO-CeO复合材料表现出更高的法拉第效率和CH的部分电流密度。原位光谱和理论计算证实，CuO-CeO复合材料中的Cu-O-Ce桥可以有效增强H吸附并稳定Cu（I）物种，促进随后的C-C偶联并进一步质子化形成CH的关键COCHO中间体。这项工作为调节H吸附和稳定Cu（I）物种以促进CO转化为C产物提供了新的见解。
