Synergistic Inhibition of Oxide Formation in Oxidation Catalysis: A First-Principles Kinetic Monte Carlo Study of NO + CO Oxidation at Pd(100)
Synergistic Inhibition of Oxide Formation in Oxidation Catalysis: A First-Principles Kinetic Monte Carlo Study of NO + CO Oxidation at Pd(100)
复制标题
DOI：
10.1021/acscatal.6b01344
复制
发表时间：
2016-07
期刊：
影响因子：
12.9
通讯作者：
Juan M Lorenzi;S. Matera;K. Reuter
中科院分区：
文献类型：
--
作者：
Juan M Lorenzi;S. Matera;K. Reuter
在富氧反应条件下氧化物的形成已经独立地报道了用Pd单晶模型催化剂的CO氧化和NO氧化。我们提出了一项第一性原理动力学蒙特卡罗研究，解决了暴露于含CO和NO进料的Pd（100）处同时发生的两种反应。即使在大多数富氧进料中，发现非常少量的NO将表面氧覆盖率降低到远低于诱导氧化物形成所需的水平。即使NO和CO竞争相同的表面位点和表面氧，进行中的NO氧化反应进一步导致CO氧化活性的部分强烈增强。这突出了多组分气体进料对表面组成和催化活性的协同效应，这些效应不能被捕获，也不能从关注单个反应的流行研究中推断出来。
Oxide formation under oxygen-rich reaction conditions has independently been reported for both CO oxidation and NO oxidation with Pd single-crystal model catalysts. We present a first-principles kinetic Monte Carlo study addressing the simultaneous occurrence of both reactions at Pd(100) exposed to CO- and NO-containing feeds. Even in most oxygen-rich feeds, very small amounts of NO are found to reduce the surface oxygen coverage well below the level required to induce oxide formation. Even though NO and CO compete for the same surface sites and surface oxygen, the ongoing NO oxidation reactions furthermore lead to a partially strong enhancement of the CO oxidation activity. This highlights synergistic effects of multicomponent gas feeds on both surface composition and catalytic activity that cannot be captured, nor extrapolated from prevalent studies focusing on individual reactions.