My doctoral research has been focused on understanding and developing novel noble metal heterogeneous catalysts for the selective aerobic oxidation of organic molecules, specifically tandem oxidative coupling of alcohols. I initially developed a Pd-based catalyst, promoted with Bi and Te, capable of oxidizing alcohols to carboxylic acids with the broadest substrate scope reported to date. This system also proved capable of exclusive conversion of alcohols to methyl ester, when run in methanol. I sought to understand the fundamental forces governing this selectivity to provide insight into how the catalyst operates. Finally, I leveraged unexpected reactivity for a catalyst I synthesized to develop the first reported Rh-based catalyst system for the aerobic oxidation of alcohols, in particular for the formation of nitriles. The significant insights and understandings resulting from my doctoral work has broader implications for the development of heterogeneous catalysts for other organic transformations.