Mediating CO2 Electroreduction Activity and Selectivity over Atomically Precise Copper Clusters

被引：123

作者：

Liu, Li-Juan ^{[1
,2
]}

Wang, Zhi-Yuan ^{[1
,2
]}

Wang, Zhao-Yang ^{[1
,2
]}

Wang, Rui ^{[1
,2
]}

Zang, Shuang-Quan ^{[1
,2
]}

Mak, Thomas C. W. ^{[1
,2
,3
,4
]}

机构：

[1] Zhengzhou Univ, Henan Int Joint Lab Tumor Theranost Cluster Mat, Green Catalysis Ctr, Henan Key Lab Crystalline Mol Funct Mat, Zhengzhou 450001, Peoples R China

[2] Zhengzhou Univ, Coll Chem, Zhengzhou 450001, Peoples R China

[3] Chinese Univ Hong Kong, Dept Chem, Shatin, Hong Kong, Peoples R China

[4] Chinese Univ Hong Kong, Ctr Novel Funct Mol, Shatin, Hong Kong, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2022年 / 61卷 / 35期

基金：

中国国家自然科学基金;

关键词：

Atomically Precise; CO2; Reduction; Copper Clusters; Structure-Activity Relationships; GOLD NANOCLUSTERS; CARBON-DIOXIDE; REDUCTION; HYDRIDE; AU; ELECTROCATALYST; EVOLUTION; CATALYSIS; SIZE; CU;

D O I：

10.1002/anie.202205626

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Atomically precise copper clusters are highly desirable catalysts for electrocatalytic CO2 reduction reaction (CO2RR) and provide an ideal platform for elaborating structure-activity relationships. However, systematic comparative studies of Cu cluster isomers for electrocatalytic CO2RR are lacking because they are challenging to synthesize. A group of structurally precise Cu-8 cluster isomers with different core structures (cube- and ditetrahedron-shaped) were developed and investigated for highly active and selective CO2 reduction. Electrocatalytic measurements showed that the ditetrahedron-shaped Cu-8 cluster exhibited a higher FEHCOOH (approximate to 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-8 clusters and decreased free energies for the adsorbed HCOO* intermediates on the ditetrahedron-shaped Cu-8 clusters.

引用

页数：7

共 59 条

[1]

[Anonymous], 2019, ANGEW CHEM, V131, P15818

[2]

[Anonymous], 2021, ANGEW CHEM, V133, P470

[3] Electrochemical CO2 Reduction: Classifying Cu Facets [J].