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

被引：121

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

页码：4981 / 4985

页数：5

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