Theoretical and Experimental Exploration of Transition Metals as Hydrogen Storage Materials with Catalytic Dehydrogenation Activity

The direct conversion of readily-available methane into useful chemicals is limited due to the molecule’s symmetry and strong C-H bonds. In this thesis, the direct upgrade of methane to desirable higher hydrocarbons is sought. Presently, the most studied method for the upgrade of methane is the oxidative coupling of methane. However, this method has failed to yield an economically viable process due to poor carbon selectivities, which result from the over-oxidation of the reactive CH3 intermediate into CO and CO2. To avoid over-oxidation, the use of hydride-forming metals is explored to catalytically cleave the C-H bond, abstract hydrogen, and form C2 species in the absence of oxygen. Theoretical and experimental results show that five early transition metals can form metal hydrides and activate the C-H bond of methane. The understanding gained through this thesis builds the foundation for future work on the utilization of metal hydrides in important reactions.