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In Situ DRIFTS Study of the Low Temperature Selective Catalytic Reduction of NO with NH_3 over MnO_x Supported on Multi-Walled Carbon Nanotubes Catalysts
並列摘要
MnO_x supported on multi-walled carbon nanotubes (MWCNTs) catalysts were prepared by the pore volume impregnation method and used for low-temperature selective catalytic reduction (SCR) of NO with NH_3. Based on the previous study, 10 wt.% loading MnO_x/MWCNTs were then selected for investigation of the reaction mechanism by in situ Diffuse Reflectance Infrared Fourier Transform spectroscopy (in-situ DRIFTS). The important intermediates in the SCR of NO_x process at 210°C were discussed based on the DRIFTS results. Furthermore, the NH_3-SCR reaction pathways over MnO_x/MWCNTs catalysts were proposed. The results showed that NH_4^+ species on Brønsted acid sites and coordinate ammonia species on Lewis acid sites existed during the SCR reaction. NH_4^+ species was more active than coordinate ammonia species over the catalysts at 210°C. Most of NO_x ad-species would react with NH_3 ad-species. However, nitrite species, bidentate and monodentate nitrates contributed to the SCR reaction over the catalysts mostly. Two possible reaction pathways were proposed. One was that NO_x ad-species could react with NH_4^+ to form intermediate of NH_4N_2O_4 (a), NH_4NO_2 (a) or NH_4NO_3 (a), then to produce N_2 and H_2O as the final products. The other pathway was that NH_3 was initially adsorbed on active site and NH_2 was formed, then NH_2 reacted with NO_x ad-species to produce intermediate NH_2NO_2 or NH_2NO_3 which were unstable and would decompose into N_2 and H_2O.
延伸閱讀
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