Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO2 Reduction to CO

被引：648

作者：

Hansen, Heine A.

Varley, Joel B.

Peterson, Andrew A.

Norskov, Jens K. ^{[1
]}

机构：

[1] Stanford Univ, Dept Chem Engn, SUNCAT Ctr Interface Sci & Catalysis, Stanford, CA 94305 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2013年 / 4卷 / 03期

关键词：

ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; GOLD ELECTRODE; MONOXIDE; HYDROCARBONS; ENERGETICS; CONVERSION; KINETICS; METHANE;

D O I：

10.1021/jz3021155

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We develop a model based on density functional theory calculations to describe trends in catalytic activity for CO2 electroreduction to CO in terms of the adsorption energy of the reaction intermediates, CO and COOH. The model is applied to metal surfaces as well as the active site in the CODH enzymes and shows that the strong scaling between adsorbed CO and adsorbed COOH on metal surfaces is responsible for the persistent overpotential. The active site of the CODH enzyme is not subject to these scaling relations and optimizes the relative binding energies of these adsorbates, allowing for an essentially reversible process with a low overpotential.

引用

收藏

页码：388 / 392

页数：5

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