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《Chinese Journal of Catalysis》 2003-05
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Mechanistic Study of Lean NO_x Reduction with Propene over Ag/Al_2O_3 by in Situ DRIFTS

YU Yunbo, HE Hong *(Research Center for Eco Environmental Sciences, The Chinese Academy of Sciences, Beijing 100085, China)  
Ag/Al 2O 3 is known as one of the most effective catalysts for the hydrocarbon selective catalytic reduction (HC SCR) of NO x . However, the HC SCR of NO x is usually suppressed in the presence of water vapor, which inevitably exists in various exhausts, resulting in a difficulty for utilization of the catalysts. Thus, it is necessary to understand the effect of water vapor on mechanistic level. The Ag/Al 2O 3 catalyst with Ag loading of 5%was prepared by the impregnation method. Al 2O 3 powder was dissolved in an appropriate amount of silver nitrate aqueous solution. The sample was dried at 393 K for 3 h and calcined at 873 K for 3 h in air. The catalyst activity test was carried out in a fixed bed reactor with a gas mixture containing 0 08% NO, 0 171?4% C 3H 6, 10 0% O 2 and a balance of N 2 at a total flow rate of 4 L/min ( W/F =0 018 g/cm 3 , GHSV= 50?000 h -1 ) in a temperature range of 473~923 K. Water vapor was supplied with a syringe pump into the gas stream and vaporized by a coiled heater set at inlet of the reactor. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) spectra were recorded on a Nexus 670 (Thermo Nicolet) FT IR equipped with an in situ diffuse reflection chamber and a high sensitivity MCT detector. Because water vapor in gas phase and adsorbed water on Ag/Al 2O 3 surface strongly absorb infrared ray, a reference spectrum of Ag/Al 2O 3 in a flow of O 2+N 2 (and water vapor, if any) was subtracted from each spectrum at the same temperature respectively. The mechanism of lean NO x reduction with C 3H 6 over Ag/Al 2O 3 was studied by in situ DRIFTS under the real reaction condition and the results are in good agreement with our previous conclusions obtained in a vacuum system, suggesting that R ONO and R NO 2 species are formed by the reactions of C 3H 6 with NO 2 and/or NO - 3 species and convert to Ag NCO and Al NCO species over the Ag/Al 2O 3 surface. This is the rate determining step in catalytic reduction of NO into N 2 in a steady state because Ag NCO and Al NCO species have very high reactivity for converting NO x and O 2 to N 2 and CO 2. The presence of water vapor suppresses the formation of R ONO and R NO 2 on the Ag/Al 2O 3 surface and thus limits the reaction rate. These results indicate that it is necessary to design a water resistant catalyst or to find an effective reductant to vary the reaction path.
【Fund】: 中国科学院百人计划;; 国家自然科学基金 (5 0 14 80 18);; 863计划(2 0 0 1AA64 3 0 40 )资助项目
【CateGory Index】: O643.3
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