Electrons to Reactors Multiscale Modeling: Catalytic CO Oxidation over RuO2
Electrons to Reactors Multiscale Modeling: Catalytic CO Oxidation over RuO2
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DOI：
10.1021/acscatal.8b00713
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发表时间：
2018-04
期刊：
影响因子：
12.9
通讯作者：
Jonathan E. Sutton;Juan M Lorenzi;J. Krogel;Q. Xiong;S. Pannala;S. Matera;A. Savara
中科院分区：
文献类型：
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作者：
Jonathan E. Sutton;Juan M Lorenzi;J. Krogel;Q. Xiong;S. Pannala;S. Matera;A. Savara
第一性原理动力学蒙特卡罗（1 p-kMC）模拟CO氧化的两个方面，RuO 2（110）和RuO 2（111），耦合到计算流体动力学（CFD）模拟包MFIX，然后进行反应堆规模的模拟。1 p-kMC与计算流体动力学耦合最近已被证明是一种可行的方法，用于将分子尺度的机理知识转化为反应器规模，从而能够与原位和在线实验测量进行比较。只有少数研究与这种耦合已经出版。这项工作将多个催化表面刻面的规模耦合模拟，并研究了三种可能性：两种可能性的每个刻面单独的反应器中的主导相，也有可能，这两个刻面都存在于催化剂颗粒上的比例预测的从头算基于武尔夫建设。当吸附物之间的横向相互作用包括在1 p-kMC模拟，两个表面，RuO 2…
First-principles kinetic Monte Carlo (1p-kMC) simulations for CO oxidation on two RuO2 facets, RuO2(110) and RuO2(111), were coupled to the computational fluid dynamics (CFD) simulations package MFIX, and reactor-scale simulations were then performed. 1p-kMC coupled with CFD has recently been shown as a feasible method for translating molecular scale mechanistic knowledge to the reactor scale, enabling comparisons to in situ and online experimental measurements. Only a few studies with such coupling have been published. This work incorporates multiple catalytic surface facets into the scale-coupled simulation, and three possibilities were investigated: the two possibilities of each facet individually being the dominant phase in the reactor, and also the possibility that both facets were present on the catalyst particles in the ratio predicted by an ab initio thermodynamics-based Wulff construction. When lateral interactions between adsorbates were included in the 1p-kMC simulations, the two surfaces, RuO2...