Low temperature catalytic NO oxidation over microporous materials
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文摘
It is shown that NO oxidation is catalyzed by chabazite zeolites in the proton (H+), sodium (Na+) and siliceous forms, by microporous carbons and by the metal-organic framework (MOF) material Basolite A100庐 at temperatures between 298 K and 423 K. Reaction orders at low conversion for NO and O2 are 2 and 1, as observed for the gas-phase reaction. At higher conversion and low temperatures, the rate decreases because of the presence of various NxOy species within the pores of the materials. Catalytic rates decrease with increasing temperature and yield negative apparent activation energies (鈭?4.9 to 鈭?7.5 kJ mol鈭?). The catalytic properties of the samples are attributed to their ability to stabilize a [N2O4]鈥?/sup> transition state within the micropores through van der Waals forces. Na-SSZ-13 samples exhibit faster catalytic rates than siliceous chabazite due to the additional presence of electrostatic forces stabilizing the transition state. An enhancement of catalytic rates on H-SSZ-13 is also observed but is the result of more complex interactions due to the formation of NO+ and in the zeolite pores that can also stabilize the [N2O4]鈥?/sup>.

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