Activation energy calculation of NO-CO reaction on rhodium surface bydensity functional theory
Activation energy calculation of NO-CO reaction on rhodium surface bydensity functional theory
复制标题
密度泛函理论计算铑表面NO-CO反应活化能
DOI：
10.1016/j.cattod.2018.07.056
复制
发表时间：
2019
期刊：
影响因子：
5.3
通讯作者：
Yukihiro Shimizu
中科院分区：
文献类型：
--
作者：
Taisei Ito;Yukihiro Shimizu
对Rh（111）表面NO-CO反应进行了密度泛函理论计算。采用爬升图像微推弹性带法研究了反应途径和反应活化能。在反应的基本步骤中，速率决定步骤是NO解离。对计算结果的详细分析，如反应过程中原子构型的快照、态的偏密度和电荷密度分布，揭示了决定NO-CO反应催化活性的因素。NO在Rh和Cu表面的吸附能差异决定了其催化活性的相对优势。表面的氧吸附能力是决定NO-CO反应催化活性的重要因素之一。O原子的强吸附抑制co2的组成，而O原子的弱吸附抑制NO的解离。在密度泛函理论计算的基础上，可以为寻找替代催化剂提供指导。
The density functional theory calculations for the NO–CO reaction on Rh(111) surface are carried out. The reaction pathway and the activation energy of the reaction are investigated by employing the climbing image nudged elastic band method. The rate determining step in the elementary steps of the reaction is the NO dissociation. Detailed analyses of the calculation results, such as the snapshot of the atomic configuration during the reaction, the partial density of states, and the charge density distribution, reveal what will decide the catalytic activities of NO–CO reaction. The difference of adsorption energies of NO on Rh and Cu surfaces causes the relative merit of the catalytic activity. The oxygen adsorption ability of the surface is one of the important factors to decide the catalytic activity of NO–CO reaction. The strong adsorption of an O atom inhibits the CO2composition, on the other hand, the weak adsorption of an O atom inhibits the NO dissociation. The guidelines for searching of the alternative catalysts can be made based on the density functional theory calculations.