Heterogeneities in the structure of active centers in metal-containing porous materials are unavoidable and complicate the description of chemical events occurring along reaction coordinates at the atomic level. Metal containing zeolites include sites of varied local coordination and secondary confining environments, requiring careful titration protocols to quantify the predominant active sites. Hybrid organometallic-zeolite catalysts are useful well-defined platform materials for spectroscopic, kinetic, and computational studies of heterogeneous catalysis that avoid the complications of conventional metal-containing porous materials. Such materials have been synthesized and studied previously, but catalytic applications were mostly limited to liquid-phase oxidation and electrochemical reactions. The hydrothermal stability, time-on-stream stability, and utility of these materials in gas-phase oxidation reactions are under-studied. The potential applications for single-site heterogeneous catalysts in fundamental research are abundant and motivate future synthetic, spectroscopic, kinetic, and computational studies.