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

该项目的目标是进行基本的结构性质研究，这将有助于合理设计催化结构，以期对感兴趣的反应具有最大的收率和选择性。将研究各种局部沸石结构的催化活性、吸附特性和固有材料性质。在涉及碳氢化合物的特定反应中，将研究以确定哪种结构对特定反应最活跃。一个重要的结果将是一个公式，将固体酸性沸石的最重要性质与沸石的相应催化活性联系起来。将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的统计力学技术。后两者结合将允许模拟任何时间尺度和任何温度下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，将进行一个实验项目来验证模拟结果。教育活动包括为本科生开设分子计算方法学研究项目，为高年级学生开设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、裂化和异构化。

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.