Hydrophobic zeolite modification for in situ peroxide formation in methane oxidation to methanol

By Zhu Jin, Liang Wang, E. Zuidema, K. Mondal, Ming Zhang, Jian Zhang, Chengtao Wang, Xiangju Meng, Hengquan Yang, C. Mesters and 1 more. Science, 2020

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Confining peroxide to make methanol In principle, hydrogen peroxide would be an efficient oxidant for the conversion of methane to methanol under mild conditions. In practice, however, it is currently too expensive to produce the peroxide ahead of time for this purpose. Jin et al. report a catalyst system that generates and concentrates hydrogen peroxide for immediate reaction with methane. A hydrophobically coated zeolite keeps the peroxide close to the gold and palladium active site, where incoming methane is then selectively oxidized to methanol. Science, this issue p. 193 A catalyst system concentrates hydrogen peroxide and methane in close proximity for efficient methanol synthesis. 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.

Subfields: Catalysis, Inorganic Chemistry, Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/5d68315ab21af8ba85d32c6f5bb1968ddf3dd9c6

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