Shao Ping, Zhou Wei, Hong Qin-Long, Yi Luocai, Zheng Lirong, Wang Wenjing, Zhang Hai-Xia, Zhang Huabin, Zhang Jian
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, P. R. China.
Department of Applied Physics, Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology, Faculty of Science, Tianjin University, Tianjin, 300072, P. R. China.
Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16687-16692. doi: 10.1002/anie.202106004. Epub 2021 Jun 18.
Fundamental understanding of the dependence between the structure and composition on the electrochemical CO reduction reaction (CO RR) would guide the rational design of highly efficient and selective electrocatalysts. A major impediment to the deep reduction CO to multi-carbon products is the complexity of carbon-carbon bond coupling. The chemically well-defined catalysts with atomically dispersed dual-metal sites are required for these C-C coupling involved processes. Here, we developed a catalyst (BIF-102NSs) that features Cl bridged dimer copper (Cu ) units, which delivers high catalytic activity and selectivity for C H . Mechanistic investigation verifies that neighboring Cu monomers not only perform as regulator for varying the reaction barrier, but also afford distinct reaction paths compared with isolated monomers, resulting in greatly improved electroreduction performance for CO .
深入理解结构和组成与电化学一氧化碳还原反应（CO RR）之间的依赖关系，将指导高效且选择性的电催化剂的合理设计。将CO深度还原为多碳产物的一个主要障碍是碳-碳键偶联的复杂性。对于这些涉及碳-碳偶联的过程，需要具有原子分散双金属位点的化学定义明确的催化剂。在此，我们开发了一种具有Cl桥连二聚体铜（Cu）单元的催化剂（BIF-102NSs），它对C₂H₄具有高催化活性和选择性。机理研究证实，相邻的Cu单体不仅作为调节反应势垒的调节剂，而且与孤立的单体相比提供了不同的反应路径，从而大大提高了CO的电还原性能。
