Theoretical Studies of Inorganic and Organometallic Systems

美国德州农工大学化学系的Michael B. Hall教授获得了美国国家科学基金会理论与计算化学项目的资助，对无机和有机金属化学中当前感兴趣的问题进行从头算理论研究，特别是均相催化。目前所采用的计算方法包括多组态自洽场和组态相互作用波函数的全梯度几何优化技术。正在进行的应用通常需要在这些可能的边界进行计算，必要时，对现有方法进行修改和改进，以便能够进行这些计算。这项资助下的工作重点是研究和表征催化反应的四个基本步骤：氧化加成；替换;migratory-insertion;原子转移。正在研究的系统包括生物和工业上重要的催化氧化过程模型。这项拨款支持的工作将有助于提供理解，使研究人员能够对涉及生物和工业过程的反应进行定性化学预测，而无需进一步计算。一个主要目标是发现和预测无机和有机金属体系的结构和反应性的系统趋势。为了实现这些目标，霍尔教授在理论上研究的系统被选择得尽可能接近实验学家所研究的系统。

Professor Michael B. Hall at the Department of Chemistry, Texas A&M University is supported by a grant from the Theoretical and Computational Chemistry Program at NSF for ab initio theoretical studies of problems of current interest in inorganic and organometallic chemistry, especially homogeneous catalysis. The computational methods which are being used involve full-gradient geometry optimization techniques for both multiconfiguration self-consistent-field and configuration interaction wavefunctions. The applications being made often require calculations at the frontier of those possible and, if necessary, the existing methods are modified and enhanced so that these calculations can be performed. The work under this grant is focused on the study and the characterization of four fundamental steps in catalytic reactions: oxidative-addition; substitution; migratory-insertion; and atom transfer. The systems being studied include models for biologically and industrially important catalytic oxidation processes. The work supported by this grant will help to provide the understanding which will allow researchers to make qualitative chemical predictions, without the need for further calculations, related to reactions involved in biological and industrial processes. A major objective is the discovery and prediction of systematic trends in the structures and reactivity of inorganic and organometallic systems. In order to achieve these objectives the systems being studied theoretically by Professor Hall are chosen to be as close as possible to systems being studied by experimentalists.