Simulation of Chemical Processes in Condensed Phases Using Hybrid Quantum and Molecular Mechanical Potentials

Jiali Gao得到了理论和计算科学基金会的资助。 化学计划继续他的混合量子的发展 机械和统计力学技术来模拟化学 在溶液和多相催化过程中。 的目标 研究目的是获得合理的定量一致性， 实验溶剂化能 该方法提供了新的见解， 分子间相互作用的性质，特别是， 极化效应对生物化学过程的贡献 以及对凝聚相感兴趣的材料。 应用涉及 α-氯醚的热分解和α-氯醚模型化合物的水解 在有机和水溶液中的糖基衍生物。 另一个主要 研究的重点是研究吸附、结合和化学作用 与使用沸石将甲醇转化为汽油有关的反应 催化作用 大多数具有商业重要性的化学过程都是在溶液中进行的。 计算机模拟溶液中的化学反应提供了重要的 分子水平的洞察力的因素，影响反应速率。 然而，许多更有趣的键断裂反应表现出 量子效应不能有效地使用经验模型 潜力高的方法涉及使用组合模拟 方法，使用蒙特卡罗和分子轨道理论来处理 量子自由度在化学过程中发生变化 反应

Jiali Gao is supported by a grant from the Theoretical and Computational Chemistry Program to continue his development of a hybrid quantum mechanical and statistical mechanical technique to simulate chemical processes in solution and in heterogeneous catalysis. The objective of the research is to obtain reasonably quantitative agreement with experimental solvation energies. The approach provides new insights on the nature of intermolecular interactions, in particular, specific contributions from the polarization effects for processes of biochemical and materials interest in condensed phases. Applications involve the thermolysis of alpha-chloroethers and hydrolysis of model compounds for glycosyl derivatives in organic and aqueous solutions. Another major thrust of the research is the study of adsorption, binding, and chemical reactions associated with methanol-to-gasoline conversion using zeolite catalysis. Most chemical processes of commercial importance take place in solution. Computer simulations of chemical reactions in solution provide important molecular level insights into the factors that influence reaction rates. Many of the more interesting bond breaking reactions, however, exhibit quantum effects that cannot be modeled effectively using empirical potentials. Gao's approach involves the use of a combined simulation approach which uses Monte Carlo and molecular orbital theory to treat the quantum degrees of freedom undergoing change during the chemical reaction.