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

国际化学合作：氮氧化物储存还原催化剂的第一原理多晶格动力学蒙特卡罗模拟

基本信息

批准号：
181861493
负责人：
Professor Dr. Karsten Reuter
金额：
--
依托单位：
Department of Chemical Engineering
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2010
资助国家：
德国
起止时间：
2009-12-31 至 2014-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/181861493?language=en
关键词：
International Collaboration Chemistry First Principles

项目摘要

The broad objective of the research is to gain a fundamental understanding of the surface reaction chemistry of exhaust catalysts operating under cycling conditions. Using an integrated theoretical approach we specifically target NOx abatement, with particular emphasis on the appearance and destruction of surface oxide phases as the reactor conditions cycle from oxidative to reductive during the operation of the NOx Storage Reduction (NSR) catalyst system. Methodologically this requires material-specific, quantitative and explicitly 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. To meet these challenging demands we will develop a novel multi-scale methodology relying on a multi-lattice first-principles kinetic Monte Carlo (kMC) approach. As representative example the simulations will be carried out on a PdO(101)/Pd(100) surface oxide model, but care will be taken to ensure a generalization of the multi-lattice first-principles kMC approach to other systems in which phase transformations may occur and result in a change in the surface lattice structure depending upon environmental variables.

这项研究的主要目的是对循环条件下废气催化剂的表面反应化学有一个基本的了解。采用综合理论方法，我们专门针对NOx减排，特别强调在NOx存储还原（NSR）催化剂系统运行期间，反应器条件从氧化到还原循环时，表面氧化相的外观和破坏。在方法上，这需要特定于材料的、定量的、明确依赖于时间的模拟工具，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，同时考虑原子尺度上的站点异质性和演化表面的空间分布。为了满足这些具有挑战性的要求，我们将开发一种基于多晶格第一性原理动力学蒙特卡罗（kMC）方法的新型多尺度方法。作为代表性的例子，模拟将在PdO(101)/Pd（100）表面氧化物模型上进行，但要注意确保将多晶格第一性原理kMC方法推广到其他系统中，在这些系统中可能发生相变并导致表面晶格结构的变化，这取决于环境变量。