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.