Atmosphere-Pressure Methane Oxidation to Methyl Trifluoroacetate Enabled by a Porous Organic Polymer-Supported Single-Site Palladium Catalyst
Yiwen Zhang, Min Zhang, Zheng‐Bo Han, Shijun Huang, Daqiang Yuan, Weiping Su
Abstract
The efficient conversion of methane into methanol at low temperature under low pressure remains a great challenge largely because of the inertness and poor solubility of methane. Herein, we report that a porous organic polymer-supported Pd catalyst, which was constructed via Friedel–Crafts type polymerization between 4,6-dichloropyrimidine and 1,3,5-triphenyl benzene and subsequent metalation, enabled the conversion of methane to methyl trifluoroacetate, a precursor to methanol, under atmosphere pressure (1 atm) at 80 °C to afford a 51% yield relative to methane with a TON of 664 over 20 h. On increasing the pressure to 30 bar, this palladium catalyst offered a TON of 1276 for a run and could be reused for at least five runs without a notable loss of activity. The characterization of this Pd catalyst revealed its good affinity for methane uptake that would increase the concentration of methane in the local space around the Pd center and the homogeneous distribution of Pd2+ on support that would protect the catalytically active metal species, shedding light on the high catalytic activity of this Pd catalyst toward methane conversion.