Pd（100）对PdO（sqrt5xsqrt5）的R27氧化：第一原理动力学Phase Diagrams和双稳态条件
CO oxidation on Pd(100) vs. PdO(sqrt5xsqrt5)R27^o: First-Principles Kinetic Phase Diagrams and Bistability Conditions
摘要：
我们提出了第一性原理动力学蒙特卡罗（1 p-kMC）模拟解决CO氧化反应在Pd（100）的气相条件下，从超高真空（UHV）到环境压力和高温。对于后一种技术相关的制度，关于活性表面的性质存在着长期的争论。原始金属表面、超薄（sqrt 5xsqrt 5）R27^0 PdO（101）表面氧化物和较厚的氧化物层均被认为是活性状态。我们调查这些假设与1 p-kMC模拟集中在Pd（100）表面或PdO（101）表面氧化物和有趣地获得一系列的（T，p）-条件，其中两个终端出现亚稳态。预测的双稳态机制很好地与Hendriksen及其同事实验报告的振荡行为联系在一起[Catal. Today 105，234（2005）]。在这个制度，我们发现，这两个表面终端表现出非常相似的内在反应性，这把怀疑试图分配催化功能，只有一个活性状态。
英文摘要：
We present first-principles kinetic Monte Carlo (1p-kMC) simulations addressing the CO oxidation reaction at Pd(100) for gas-phase conditions ranging from ultra-high vacuum (UHV) to ambient pressures and elevated temperatures. For the latter technologically relevant regime there is a long-standing debate regarding the nature of the active surface. The pristine metallic surface, an ultra-thin (sqrt5xsqrt5)R27^o PdO(101) surface oxide, and thicker oxide layers have each been suggested as the active state. We investigate these hypotheses with 1p-kMC simulations focusing on either the Pd(100) surface or the PdO(101) surface oxide and intriguingly obtain a range of (T, p)-conditions where both terminations appear metastable. The predicted bistability regime nicely ties in with oscillatory behavior reported experimentally by Hendriksen and coworkers [Catal. Today 105, 234 (2005)]. Within this regime we find that both surface terminations exhibit very similar intrinsic reactivity, which puts doubts on attempts to assign the catalytic function to just one active state.
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