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Reactive Trapping of Dilute Methane Emissions by Surface Oxygen Intermediates on Copper Zeolites for Total Oxidation
Jing Ma1, Dieter Plessers1, Laura D Elmendorf2
1Department of Microbial and Molecular Systems, Center for Sustainable Catalysis and Engineering, KU Leuven, 3001 Leuven, Belgium.
Abstract:
Through reactive trapping, Cu-zeolites are shown to catalytically remove methane at 2 ppm, oxidizing it to CO2 in air at 350 °C. Partial reaction orders are 0.56-0.75 in CH4 and quasi-zero in O2. Together with kinetic analysis of reaction steps in O2 activation, this indicates that, along with the first CH4 reaction step, O-O bond breakage is also kinetically relevant, presenting a useful catalyst design target. Among tested zeolites, CuNaMFI (Si/Al = 14.3, Cu/Al = 0.53) exhibits optimal performance and stability, especially through low Brønsted acidity and its formation of dispersed Cu2+/O species that perform oxidative trapping of dilute methane.
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