CAREER: First-Principles Dynamic Studies of Solid-Acid Zeolite Catalysis: Structure-Property Relationships and Catalyst Design

这个项目的目标是进行基本的结构-性质研究，这些研究将有助于合理设计预期具有最大产率和感兴趣反应的选择性的催化结构。我们将研究各种局部沸石结构的催化活性、吸附特性和本征材料性质。特别是，将对涉及碳氢化合物的反应进行调查，以确定哪些结构对特定反应最活跃。一个主要结果将是一种将固体酸沸石的最重要性质与沸石的相应催化活性联系起来的配方。采用的基本方法是密度泛函理论、Car-Parinello分子动力学和最近发展起来的统计力学技术。后两者的结合将允许在任何温度下模拟任何时间尺度的催化活化的化学过程。通过麻省理工学院和其他组织的合作，将进行一项实验计划，以验证模拟的结果。教育举措包括为本科生开发分子计算方法学的研究计划，以及为高年级学生开发一门专注于量子力学方法的新课程。这项工作将应用于基本的化学过程，如碳氢化合物合成、脱水、裂解和异构化。

The goal of this project is to perform fundamental structure-property research that will be useful in the rational design of catalytic structures anticipated to have maximum yield and selectivity for reactions of interest. Catalytic activity, adsorption characteristics, and intrinsic material properties of a variety of local zeolite structures will be studied. In particular reactions involving hydrocarbons will be investigated to determine which structures are most active for a particular reaction. A major result will be a formulation that relates the most important properties of solid acid zeolites to the corresponding catalytic activity of the zeolite. The basic methodologies to be employed are density functional theory, Car-Parinello molecular dynamics, and recently developed statistical mechanical techniques. The latter two combined will allow the simulation of catalytically activated chemical processes of any time scale at any temperature. Through collaborations at MIT and other organizations, an experimental program to validate the results of the simulations will be carried out. Educational initiatives include the development of a research program in molecular computational methodology for undergraduates and a new course for seniors that will focus on quantum mechanical methods. This work will have application to essential chemical processes such as hydrocarbon synthesis, dehydration, cracking, and isomerization.