Activating a Low Overpotential CO2 Reduction Mechanism by a Strategic Ligand Modification on a Ruthenium Polypyridyl Catalyst

被引：76

作者：

Johnson, Ben A. ^{[1
]}

Maji, Somnath ^{[1
]}

Agarwala, Hemlata ^{[1
]}

White, Travis A. ^{[1
]}

Mijangos, Edgar ^{[1
]}

Ott, Sascha ^{[1
]}

机构：

[1] Uppsala Univ, Dept Chem, Angstrom Lab, Box 523, S-75120 Uppsala, Sweden

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2016年 / 55卷 / 05期

基金：

瑞典研究理事会;

关键词：

carbon dioxide reduction; electrocatalysis; overpotential; reaction mechanisms; ruthenium; CARBON BOND FORMATION; ELECTROCATALYTIC REDUCTION; WATER-OXIDATION; ELECTROCHEMICAL REDUCTION; MULTIELECTRON REDUCTION; TRANSITION-METALS; LIQUID FUELS; DIOXIDE; COMPLEXES; MACROCYCLES;

D O I：

10.1002/anie.201508490

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The introduction of a simple methyl substituent on the bipyridine ligand of [Ru(tBu(3)tpy)(bpy)(NCCH3)](2+) (tBu(3)tpy = 4,4',4''-tri-tert-butyl-2,2':6',2''-terpyridine; bpy = 2,2'-bipyridine) gives rise to a highly active electrocatalyst for the reduction of CO2 to CO. The methyl group enables CO2 binding already at the one-electron reduced state of the complex to enter a previously not accessible catalytic cycle that operates at the potential of the first reduction. The complex turns over with a Faradaic efficiency close to unity and at an overpotential that is amongst the lowest ever reported for homogenous CO2 reduction catalysts.

引用

页码：1825 / 1829

页数：5

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