Synthetic and Mechanistic Studies of High Valent Organotransition Metal Compounds

在这个由无机，生物无机和 有机化学程序，约翰E。加州的伯考- 奥尼亚理工学院将研究合成 新型双氧相容跃迁的性质 能够选择性氧化 芳香烃.这项研究的最终目的是开发一种 用于从煤转化烃的有用的催化方法， 石油或天然气源转化为醇（特别是， 甲烷转化为甲醇），其可能更易于运输 和有用的能源或化学原料。 本项目主要有两个方向：（1）合成新的可溶性羰基化合物 或钌的过氧衍生物， 将烯烃转化为环氧化物或羰基化合物， 碳到醇，和（2）机制研究，其中涉及 碳-氧键形成或碳-氧键断裂. 铪和钽。后一个项目将导致 了解动力学和热力学因素 影响碳-氧和氢-氧键的形成. 过渡金属中心，这将有助于设计的 催化剂部分（1）。还提出了相关的研究， 可以提供一些模型化合物和转化， 与催化加氢脱硫化学相关。

In this project supported by the Inorganic, Bioinorganic and Organometallic Chemistry Program, John E. Bercaw of the Calif- ornia Institute of Technology will investigate the synthesis and properties of new types of dioxygen-compatible transition metal compounds which may be capable of selectively oxidizing hydrocarbons. The eventual aim of this research is to develop a useful catalytic method for converting hydrocarbons from coal, petroleum or natural gas sources to alcohols (in particular, methane to methanol), which may be more readily transportable and useful energy sources or chemical feedstocks. The project has two thrusts: (1) synthesis of new soluble oxo or peroxo derivatives of ruthenium, which could smoothly convert olefins to epoxides or carbonyl compounds and hydro- carbons to alcohols, and (2) mechanistic studies which involve carbon-oxygen bond formation or carbon-oxygen bond cleavage at hafnium and tantalum. The latter project would lead to an understanding of the kinetic and thermodynamic factors influencing carbon-oxygen and hydrogen-oxygen bond formation at transition metal centers which would aid in design of the catalysts in part (1). Related studies are also proposed which could provide some model compounds and transformations of relevance to catalytic hydrodesulfurization chemistry.