FUNCTIONAL MODELS FOR MMOH--REACTIVITY AND MECHANISM

结构特征与功能的相关性 甲烷单加氧酶（MMO）仍有待阐明。 大多数模型 MMO羟化酶（MMOH）的研究主要集中在结构上 和物理性质，不太强调分子氧反应性， 而对底物氧化反应的系统报道较少。 的 研究建议是针对新的二铁（II）的发展， 复杂系统作为MMOH的功能模型，基于统一的 提出了羟基化机理。 该方法首先从 双核配体体系的构建 卟啉单元，预期不仅作为间隔基用于 通过氧化还原性质完成所需反应 金属卟啉 单个分子中的两个铁（II）中心 具有一定的距离和配位位点， 用于反应性研究，包括双氧反应， 随后底物氧化，特别是甲烷转化。 一 将构建Si支撑的二铁络合物系统以模拟 蛋白质框架保护反应性的生物系统 在金属活性位点中形成的中间体，防止它们的 通过涉及其他金属络合物的双分子途径分解。 这项建议的长期目标是确定一个高效率、 用于将甲烷转化为甲醇的催化体系， 在温和的条件下，通过详细的 MMO体系的热力学和动力学机理研究。 是 我希望这项研究的结果将在一个充满希望的世界上， 那里的环境污染是一个主要问题。

The correlation between the structural features and the function of methane monooxygenase (MMO) remains to be elucidated. Most of model studies of MMO hydroxylase (MMOH) have focused primarily on structure and physical properties, with less emphasis on dioxygen reactivity, and few system was reported on the substrate oxidation reactions. The research proposal is directed toward the development of new diiron(II) complex system as functional models for MMOH, based on a unifying hydroxylation mechanism proposed. The approach begins with the construction of a dinuclear coordination ligand system with a porphyrin unit that is expected to serve as not only a spacer for the completion of the desired reaction by virtue of the redox properties of metalloporphyrins. The two iron(II) centers in a single molecule separated with certain distance and possessing coordination sites will be used for reactivity studies including dioxygen reaction and subsequent substrate oxidation, especially methane conversion. A Si-supported diiron complex system will be constructed to mimic the biological system in which the protein framework protects reactive intermediates formed in the metal active sites, preventing their decomposition by bimolecular pathways involving other metal complexes. The long-term objective of this proposal is to identify an efficient, catalytic system for the conversion of methane to methanol using dioxygen as an oxidant under mild conditions through detailed thermodynamic and kinetic-mechanistic studies of MMO system. It is hoped that the outcome of this study will be promising in a world where environmental pollution is a major concern.