International Collaboration in Chemistry: First Principles Multi-Lattice Kinetic Monte Carlo Simulations of NOx Storage Reduction Catalysts

伊利诺伊大学芝加哥分校的Randall Meyer教授得到化学系化学催化项目和国际科学与工程办公室的支持，与慕尼黑工业大学的Karsten罗伊特教授合作开展研究，开发一种结合DFT和多晶格第一性原理动力学Monte Carlo（kMC）的综合多尺度理论方法。方法，以获得在氧化和还原环境之间的循环条件下操作的排气催化剂的表面反应化学的基本理解。 要研究的具体应用是NOx储存还原（NSR）催化剂系统的PdO（101）/Pd（100）表面。 将开发特定材料和随时间变化的模拟工具，这些工具可以在NSR周期的宏观时间尺度上跟踪系统的演变，同时考虑原子尺度的站点异质性和不断变化的表面的空间分布。罗伊特教授由德国资助机构DFG资助。从基本催化的观点来看，以原子级分辨率和在排气系统操作的循环的时间尺度上跟踪表面形态的演变的能力是重要的。 所提出的方法也可能影响其他多相催化系统的模拟。它还将具有重要的实际应用，例如在汽车燃料经济性方面。 学生将接受计算催化方面的培训，并将通过学生交流计划接触国际研究经验，并有机会与德国的研究人员建立联系。

Professor Randall Meyer of the University of Illinois at Chicago is supported by the Chemical Catalysis Program in the Division of Chemistry and the Office of International Science and Engineering to conduct research in collaboration with Professor Karsten Reuter of the Technical University of Munich to develop an integrated multi-scale theoretical approach combining DFT and a multi-lattice first-principles kinetic Monte Carlo (kMC) approach to gain a fundamental understanding of the surface reaction chemistry of exhaust catalysts operating under cycling conditions between oxidizing and reducing environments. The specific application to be investigated is the PdO (101)/Pd (100) surface for the NOx storage reduction (NSR) catalyst system. Material-specific and time-dependent simulation tools that can follow the evolution of the system over the macroscopic time-scales of NSR cycles, while simultaneously accounting for the atomic-scale site heterogeneity and spatial distributions at the evolving surface, will be developed. Professort Reuter is funded by the German funding agency, the DFG. The ability to follow the evolution of surface morphology with atomic-level resolution and at the timescale of a cycle of the exhaust system operation is important from a fundamental catalysis point of view. The proposed methodology is likely to impact simulations of other heterogeneous catalytic systems as well. It will also have important practical applications, such as in automotive vehicles fuel economy. Students will be trained in computational catalysis and will be exposed to an international research experience with opportunities to network with researchers in Germany through a student exchange plan.