调控原子精确的铜簇上一氧化碳电还原活性和选择性
Mediating CO Electroreduction Activity and Selectivity over Atomically Precise Copper Clusters.
作者信息
Liu Li-Juan, Wang Zhi-Yuan, Wang Zhao-Yang, Wang Rui, Zang Shuang-Quan, Mak Thomas C W
机构信息
Henan Key Laboratory of Crystalline Molecular Functional Materials, Henan International Joint Laboratory of Tumor Theranostical Cluster Materials, Green Catalysis Center, College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China.
Department of Chemistry and Center of Novel Functional Molecules, The Chinese University of Hong Kong, Shatin, New Territories, Hong Kong SAR, China.
出版信息
Angew Chem Int Ed Engl. 2022 Aug 26;61(35):e202205626. doi: 10.1002/anie.202205626. Epub 2022 Jul 14.
Atomically precise copper clusters are highly desirable catalysts for electrocatalytic CO reduction reaction (CO RR) and provide an ideal platform for elaborating structure-activity relationships. However, systematic comparative studies of Cu cluster isomers for electrocatalytic CO RR are lacking because they are challenging to synthesize. A group of structurally precise Cu cluster isomers with different core structures (cube- and ditetrahedron-shaped) were developed and investigated for highly active and selective CO reduction. Electrocatalytic measurements showed that the ditetrahedron-shaped Cu cluster exhibited a higher FE (≈92 %) at -1.0 V and higher selectivity than the cube-shaped cluster. Theoretical investigations revealed different levels of competitiveness with the hydrogen evolution reaction on the respective core-shaped Cu clusters and decreased free energies for the adsorbed HCOO* intermediates on the ditetrahedron-shaped Cu clusters.
原子精确的铜簇是电催化CO还原反应（CO RR）非常理想的催化剂，并为阐述构效关系提供了一个理想的平台。然而，由于合成具有挑战性，目前缺乏对用于电催化CO RR的铜簇异构体的系统比较研究。开发了一组具有不同核心结构（立方和双四面体形状）的结构精确的铜簇异构体，并研究了它们用于高活性和选择性CO还原的性能。电催化测量表明，双四面体形状的铜簇在-1.0 V时表现出更高的FE（≈92%），并且比立方形状的簇具有更高的选择性。理论研究揭示了各自核心形状的铜簇上与析氢反应的不同竞争水平，以及双四面体形状的铜簇上吸附的HCOO*中间体的自由能降低。
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