Rh(100)和Rh(111)上NO-CO反应机理的动力学蒙特卡罗模拟
Kinetic Monte Carlo Modeling for the NO-CO Reaction Mechanism on Rh(100) and Rh(111).
作者信息
Liu Jiangyue, Tan Lu, Huang Liangliang, Wang Qi, Liu Yingchun
机构信息
Department of Chemistry, Zhejiang University, Hangzhou 310027, People's Republic of China.
School of Chemical, Biological & Materials Engineering, University of Oklahoma, Norman, Oklahoma 73019, United States.
出版信息
Langmuir. 2020 Mar 31;36(12):3127-3140. doi: 10.1021/acs.langmuir.9b03720. Epub 2020 Mar 16.
The NO-CO reaction on Rh(100) and Rh(111) is a prototypical catalytic system with various practical applications, including the treatment of automotive gas exhausts. With parameters derived from first-principles calculations, the Brønsted-Evans-Polanyi (BEP) relation for the reaction steps of NO-CO on Rh(100) and Rh(111) surfaces is fitted, which is more accurate and practical for the calculation of the effect of interaction between adsorbates on activation energy compared to the basic BEP relation. Further, a kinetic Monte Carlo (kMC) model for the NO-CO reaction systems on Rh(100) and Rh(111) is constructed for the exploration of the system's reaction mechanism. Besides the temperature and pressure, the coverage and activation sites are essential factors for reaction kinetic of the NO-CO reaction system. Our results are beneficial for designing more efficient, economical, and environmentally friendly next-generation catalysts.
Rh(100)和Rh(111)上的NO-CO反应是一个具有多种实际应用的典型催化体系，包括汽车尾气处理。利用第一性原理计算得出的参数，拟合了Rh(100)和Rh(111)表面上NO-CO反应步骤的布朗斯特-埃文斯-波拉尼（BEP）关系，与基本BEP关系相比，该关系在计算吸附质之间的相互作用对活化能的影响方面更准确、更实用。此外，构建了Rh(100)和Rh(111)上NO-CO反应体系的动力学蒙特卡罗（kMC）模型，以探索该体系的反应机理。除了温度和压力外，覆盖度和活化位点是NO-CO反应体系反应动力学的重要因素。我们的结果有助于设计更高效、经济和环保的下一代催化剂。
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