Selective Catalytic Oxidation of Methanol on Pt-modified Cu/SSZ-13 Zeolites: A Strategy to Change the Catalytic Performance by Impregnation Sequential
摘要
The use of methanol as an alternative fuel for marine diesel engines increases unregulated CH3OH emissions. A series of Pt-modified Cu/SSZ-13 catalysts were prepared using different impregnation method, which selectively catalyzed oxidation of CH3OH (CH3OH-SCO) to CO2 and H2O. Activity tests showed that Cu/Pt/SSZ-13 catalyst (Pt impregnated first, followed by Cu) displayed exceptional CH3OH-SCO performance, achieving 100% methanol conversion at 150 °C with negligible CO and HCHO byproduct formation (< 5 ppm) across the tested temperature range. Additionally, Cu/Pt/SSZ-13 catalyst exhibited excellent SO2 resistance and high synergistic activity for simultaneous CH3OH and NOx removal. Characterization results demonstrated that Cu/Pt/SSZ-13 catalyst exhibited larger pore size, higher specific surface area, abundant strong alkaline site density and elevated surface-adsorbed oxygen (Oads) proportion. It was originated from the preferential introduction of Pt and subsequent doping of Cu enhanced the synergistic interaction at the interface of PtOx and CuO species, which facilitated the rapid migration of reactive oxygen species, thus accelerating the methanol dehydrogenation and deep oxidation. In-situ DRIFTS results indicated that Cu/Pt/SSZ-13 inhibited the deposition of formate while promoting the rapid conversion of intermediates such as formaldehyde and formic acid to CO2.
Graphical Abstract