Selective partial oxidation of methane to methanol suffers from low efficiency. Here, we report a heterogeneous catalyst system for enhanced methanol productivity in methane oxidation by in situ generated hydrogen peroxide at mild temperature (70°C). The catalyst was synthesized by fixation of AuPd alloy nanoparticles within aluminosilicate zeolite crystals, followed by modification of the external surface of the zeolite with organosilanes. The silanes appear to allow diffusion of hydrogen, oxygen, and methane to the catalyst active sites, while confining the generated peroxide there to enhance its reaction probability. At 17.3% conversion of methane, methanol selectivity reached 92%, corresponding to methanol productivity up to 91.6 millimoles per gram of AuPd per hour.
Homogeneous catalysts usually show higher catalytic activities than heterogeneous catalysts because of their high dispersion of catalytically active sites. We demonstrate here that heterogeneous catalysts of ionic liquids functionalized on superhydrophobic mesoporous polymers exhibit much higher activities in transesterification to form biodiesel than homogeneous catalysts of the ionic liquids themselves. This phenomenon is strongly related to the unique features of high enrichment and good miscibility of the superhydrophobic mesoporous polymers for the reactants. These features should allow the design and development of a wide variety of catalysts for the conversion of organic compounds.
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