The catalytic functionalization of unreactive small molecules such as methane via C-H activation is a long-standing goal in organometallic chemistry. Late transition metals, such as platinum, have been shown to be quite effective in breaking strong C-H bonds. Recently, we have been exploring the feasibility of catalytic methane functionalization employing aryl halides as oxidants. Key challenges include the unreactive nature of Pt(II) toward intermolecular aryl halide oxidative addition, and the challenges with balancing the preference for Pt(II) versus Pt(IV) oxidation states. We have recently discovered Pt(II) complexes that are capable of intermolecular oxidative addition of aryl halides under ambient conditions. We have also designed and developed new hemilabile P,N ligands that facilitate both oxidative addition and reductive elimination relative to more conventional N,N or P,P ligands. Notably, only the P,N ligands with significant steric bulk at phosphorus were capable of forming the strained chelates. These results will be discussed in the context of our ongoing efforts to catalytically functionalise methane.

Kinetic and mechanistic understanding of oxidative addition and reductive elimination of Pt(II) and Pt(IV) complexes

2019 Spring National Meeting

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