Reactions of Acidic Dinuclear Molybdenum Complexes

硫化钼络合物的反应化学在将原油转化为精炼产品所需的化学加工中占有重要地位。以硫化钼为催化剂的加氢精制原油脱硫、提高原料产品质量的工艺。该项目的目标是开发用于小分子氢解的阳离子钼络合物的氢活化能力。特别是，将研究钼络合物在氢气气氛下的反应活性，底物包括腈、异腈、氰离子、氮气、一氧化碳和芳香族杂环。拟议的研究是基于对其中一些分子进行的有希望的初步结果。对这些分子进行还原的合成体系的表征可以为开发重要的新型催化剂提供基础。这项工作也很有意义，因为它似乎从根本上定义了均相体系中硫化和氢化硫化配体的反应化学。这些可溶的络合物为硫化钼表面催化的反应，包括商业上重要的加氢脱硫反应，提供了独特的相关功能模型。这些研究也可能为理解酶中金属硫位催化还原的机理特征提供基础。

The reaction chemistry of molybdenum sulfide complexes is important in the chemical processing, required to convert crude oil to refined products. The process of hydrotreating crude oil to remove sulfur and to upgrade feedstock product quality uses molybdenum sulfide as a catalyst. The objective of the proposed project is to develop the hydrogen activating capabilities of cationic molybdenum complexes for application in the hydrogenolyses of small molecules. In particular, the reactivity of the molybdenum complexes under a hydrogen atmosphere will be investigated with substrates such as nitriles, isonitriles, cyanide ion, dinitrogen, carbon monoxide, and aromatic heterocycles. The proposed studies are based on promising preliminary results with some of these molecules. The characterization of synthetic systems which carry out the reductions of these molecules could provide the basis for the development of important new catalysts. The work is also significant because it appears to define fundamentally new reaction chemistry for sulfido and hydrosulfido ligands in homogeneous systems. The soluble complexes are proposed to provide uniquely relevant functional models for reactions catalyzed by molybdenum sulfide surfaces, including the commercially important hydrodesulfurization reactions. The studies may also provide a basis for understanding mechanistic features of reductions catalyzed by metallosulfur sites in enzymes.