Oxometal Complexes and Redox Chemistry

本研究的重点是聚氧乙烯酸盐的使用， 其他无机氧代金属物种，它们本身是 抗氧化，催化氧化还原转化， 低反应性的有机化合物，如烷烃。的 当前的目标是建立稳定的根源， 这些催化烃官能化体系的特征， 确定的机制和结构反应性的特点， 这些过程的动力学，光谱和结构 问题研究 这些新的聚氧乙烯基催化剂 光化学过程在以下方面具有潜在的实用性： 不仅是烷烃的官能化， 和储存辐射能。这项工作应该导致 现有流程的改进， 光谱现象和新催化剂的开发 流程. 均相催化烃有两种类型 基于聚氧乙烯酸酯的官能化方法。的 首先涉及烷烃的光化学官能化， 并将潜在有用的合成转化与 光到化学能的同时转换。 的 第二个涉及氧代和相关基团的热转移 转化为碳氢化合物。物理、光化学和 最近记录的几个 各种有机基质之间的相互作用， 聚氧乙烯酸盐将探测皮秒和其他 光谱研究、X射线晶体学和光化学 这些实验预计将进一步产生 关于可溶性金属氧化合物的潜在应用的信息 物种的氧化还原转化的有机和无机 分子。

The focus of this research is the use of polyoxometalates and other inorganic oxometal species, which are themselves resistant to oxidation, to catalyze redox transformations of organic compounds of low reactivity, such as alkanes. The immediate goals are to establish the origins of the stability of these catalytic hydrocarbon functionalization systems and to determine the mechanistic and structure-reactivity features of these processes by kinetics, spectroscopic and structural studies. These new polyoxometalate-based catalytic photochemical processes are of potential utility with respect to not only alkane functionalization but also the conversion and storage of radiant energy. The work should lead to improvements in the existing processes, delineation of new spectroscopic phenomena, and development of new catalytic processes. There have been two types of homogeneous catalytic hydrocarbon functionalization processes based on polyoxometalates. The first involves the photochemical functionalization of alkanes, and coupling potentially useful synthetic transformations with the simultaneous conversion of light into chemical energy. The second involves the thermal transfer of oxo and related groups into hydrocarbons. The physical, photochemical and photophysical attributes of several recently documented interactions between various classes of organic substrates and polyoxometalates will be probed by picosecond and other spectroscopic studies, X-ray crystallography and photochemical experiments.These experiments are expected to yield further information on the potential applications of soluble oxometal species to redox transformations of organic and inorganic molecules.