Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO2 Reduction to CO
Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO2 Reduction to CO
复制标题
DOI：
10.1021/jz3021155
复制
发表时间：
2013-02-07
影响因子：
5.7
通讯作者：
Norskov, Jens K.
中科院分区：
文献类型：
--
作者：
Hansen, Heine A.;Varley, Joel B.;Norskov, Jens K.
我们建立了一个基于密度泛函理论计算的模型，用反应中间产物CO和COOH的吸附能来描述CO2电还原为CO的催化活性的变化趋势。该模型被应用于金属表面以及CODH酶的活性中心，结果表明金属表面吸附的CO和吸附的COOH之间的强烈结垢是导致持续过电位的原因。CODH酶的活性位置不受这些比例关系的影响，并优化了这些吸附物的相对结合能，允许以低过电位进行基本上可逆的过程。
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.