Our research group addresses the design, synthesis, and structural/mechanistic characterization of inorganic solids useful as catalysts for chemical reactions relevant to producing, converting, and using energy carriers, to sustainable petrochemical syntheses, and to the protection of the environment. Our approach exploits novel synthetic protocols to assemble active nanostructures and single-site catalysts within porous structures and spectroscopic and titration methods to probe their atomic connectivity and electronic properties. We assess their mechanism of function through kinetic and isotopic methods of analysis, in situ spectroscopy, and density functional theory to determine the identity and kinetic relevance of elementary steps at conditions of catalysis practice. The relevance of these fundamental inquiries is evident from many patents, some of which provide enabling features in the practice of alkane CO2 valorization, zeolite-mediated organic reactions, and syntheses of chemicals with smaller environmental footprints, as well as in efficient transformations of biogenic sources of carbon into chemicals and energy carriers.