The use of molecular oxygen as a stoichiometric reoxidant in combination with a catalytic metal has exceptional practical advantages for applications in organic synthesis. We have investigated the design and development of new palladium catalysts for the aerobic oxidations of alcohols. The scope and mechanistic details of these new catalysts will be discussed. Additionally, we have recently expanded these catalytic systems to various olefin functionalization reactions where the combination of ligand and oxidant allow for entry into unique transformations. The mechanistic implications and potential applications will be discussed.