We report here results of our current work directed toward the development of first-of-its-kind organoplatinum catalysts for selective aerobic methane conversion to CH3X products (X = OH, CF3CO2). Our platinacyclic complexes are derived from two sulfonated CNN-pincer pre-ligands HL1 and HL2. The derived (L)PtII(H2O), K[(L)PtIIMe] and diastereoisomeric (L)PtIVMe(OH) have been prepared. The reactivity of these complexes toward X-H bond donors ((L)PtII(H2O); X = C, Si), toward O2 (K[(L)PtIIMe]), as well as their reductive elimination reactivity to form C-O and C-C bonds (diastereoisomeric (L)PtIVMe(OH)) have been studied. Based on the observed reactivity trends and our DFT modeling of these reactions, we propose plausible mechanisms for the reactions studied. Some tools that would allow to control the reactivity and direct the overall reaction toward selective aerobic CH4-to-CH3X transformations are proposed. This work demonstrates the potential of our novel Pt complexes supported by the sulfonated pincer ligands to carry out aerobic functionalization of methane at a Pt center.

Novel platinum complexes supported by sulfonated CNN pincer ligands relevant to aerobic methane functionalization

ACS Fall 2021

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