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教授得到化学系和国际科学与工程办公室化学催化计划的支持，与慕尼黑工业大学的Karsten Reuters教授合作开展研究，将DFT和多晶格第一原理动力学蒙特卡罗(KMC)方法相结合，开发了一种集成的多尺度理论方法，以基本了解在氧化和还原环境之间循环条件下运行的废气催化剂的表面反应化学。研究的具体应用是用于NOx储存还原(NSR)催化剂体系的PdO(101)/Pd(100)表面。将开发特定于材料和依赖于时间的模拟工具，这些工具可以在NSR循环的宏观时间尺度上跟踪系统的演变，同时考虑到原子尺度的场地异质性和演变表面的空间分布。路透教授是由德国资助机构DFG资助的。从基本催化的观点来看，能够以原子级别的分辨率并在排气系统运行的一个周期的时间尺度上跟踪表面形态的演变是重要的。所提出的方法可能也会影响其他多相催化体系的模拟。它还将有重要的实际应用，如在汽车燃油经济性方面。学生将接受计算催化方面的培训，并将接触到国际研究经验，并有机会通过学生交流计划与德国的研究人员建立网络。

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.