Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry

被引：120
|
作者：
Cao, Zhi [1 ]
Derrick, Jeffrey S. [1 ,3 ]
Xu, Jun [4 ]
Gao, Rui [5 ,6 ]
Gong, Ming [1 ,3 ]
Nichols, Eva M. [1 ,3 ]
Smith, Peter T. [1 ,3 ]
Liu, Xingwu [5 ,6 ]
Wen, Xiaodong [5 ,6 ]
Coperet, Christophe [4 ]
Chang, Christopher J. [1 ,2 ,3 ]
机构：
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[2] Univ Calif Berkeley, Howard Hughes Med Inst, Dept Mol & Cell Biol, Berkeley, CA 94720 USA
[3] Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA
[4] ETH, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1-5, CH-8093 Zurich, Switzerland
[5] Chinese Acad Sci, Inst Coal Chem, Taiyuan 030001, Shanxi, Peoples R China
[6] Synfuels China, Beijing 100195, Peoples R China
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2018年 / 57卷 / 18期
基金：
美国国家科学基金会; 中国国家自然科学基金;
关键词：
CO2; reduction; electrocatalysis; N-heterocyclic carbenes; palladium; surface chemistry; SELF-ASSEMBLED MONOLAYERS; RUTHENIUM NANOPARTICLES; GOLD NANOPARTICLES; PINCER COMPLEXES; PALLADIUM NANOPARTICLES; FORMIC-ACID; CATALYSTS; WATER; STABILIZATION; SELECTIVITY;
D O I：
10.1002/anie.201800367
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO2 reduction. Palladium functionalized with a chelating tris-N-heterocyclic carbene (NHC) ligand (Pd-timtmb(Me)) exhibits a 32-fold increase in activity for electrochemical reduction of CO2 to C1 products with high Faradaic efficiency (FEC1=86%) compared to the parent unfunctionalized Pd foil (FE=23%), and with sustained activity relative to a monodentate NHC-ligated Pd electrode (Pd-mimtmb(Me)). The results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular-materials interfaces enabled by surface organometallic chemistry.
引用
收藏
页码：4981 / 4985
页数：5
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