Synthetic, Structural and Mechanistic Investigations of High Oxidation State Organotransition Metal Compounds

这个无机、生物无机和有机金属项目的奖项为加州理工学院化学系的John E. Bercaw博士的研究项目提供了持续的支持。重点研究有机金属化合物的反应机理。碳氢化合物和其他有机底物的选择性催化氧化将被详细研究。将着重讨论影响C-O、H-O、M-O或M=O键形成和裂解的动力学和热力学因素，以及C-H键的1,2加成反应。钽的环戊二烯基化合物和含有辅助性O，O，O三足配体的高价钌和铁氧化合物将被使用。将甲烷和其他轻烷烃转化为液体，如醇或高级碳氢化合物，可以简化这些能源的运输，并使其转化为特种化学产品的第一步成为可能。通过开发能够氧化有机底物的新型过渡金属化合物，以及更好地了解在这些反应中起作用的动力学和热力学因素，可以开发出改进的氧化催化剂。在这些基础研究的过程中，将合成新的化合物，并对氧化反应的步骤进行仔细的研究。

This award in the Inorganic, Bioinorganic, and Organometallic Program provides continued support for the research program of Dr. John E. Bercaw of the Chemistry Department, California Institute of Technology. The research will focus on the mechanisms of reactions of organometallic compounds. Selective catalytic oxidation of hydrocarbons and other organic substrates will be investigated in detail. Kinetic and thermodynamic factors which influence the formation and cleavage of C-O, H-O, and M-O or M=O bonds will be emphasized, as well as 1,2 addition reactions to C-H bonds. Cyclopentadienyl compounds of tantalum and high valent ruthenium and iron oxo compounds which contain ancilliary O,O,O-tripodal ligands will be used. %%% Conversion of methane and other light alkanes to liquids, such as alcohols or higher hydrocarbons, could simplify transport of these energy sources and enable the first step of their conversion to specialty chemical products. By developing new types of transtion metal compounds which are capable of oxidizing organic substrates and providing a better understanding of the kinetic and thermodynamic factors operative in these reactions, improved oxidation catalysts may be developed. During the course of these fundamental studies, new compounds will be synthesized and careful investigations of the steps of the oxidation reactions will be carried out.