摘要
A series of silver-doped cerium zirconium oxide(Ag-CevZr)samples was synthesized successfully for selective catalytic reduction of nitric oxide(NO)with hydrogen and propene(H2/C3H6-SCR)under excess oxygen condition.The catalytic activity test proved that Ag-Ce0.4Zr exhibited the best C3H6-SCR activity.Hydrogen(H2)significantly enlianced NO conversion and widened the temperature window.Multi-technology characterizations were conducted to ascertain the properties of fabricated catalysts including X-ray diflraction(XRD),Fourier transform infrared spectrometry(FTIR),scanning electron microscopy(SEM)and H2 temperature programmed reduction(H2-TPR).In situ FTIR results demonstrated that various types of nitrates and chelating nitrite were generated on Ag-CexZr after introduction of NO.Besides,adding H2 could increase the concentration of bidentate nitrate and chelated bidentate nitrate dramatically,especially for Ce0.4Zr catalyst.Transient reaction between pre-adsorbing NO and C3H/C3H6+H2 illuminated that the most active intermediate was chelating nitrite,which was promoted significantly by H2 participation.Furthermore,adding H2 improved the formation of organo-nitro(R-N02),which was the key intennediate in C3H6-SCR.The reaction mechanism over Ag-CexZr catalysts was proposed at 200℃ as follows:nitric oxide(NO)+pr opene(C 3H6)+hy dr ogen(H2)+oxy gen(O2)→chelating nitrite (N O2-)+acry late-type species(CxHyOz)→organo-nitro(R-NO2)→isocyanate(-NCO)+cyanide(—CN)→nitrogen(N2).
基金
Supported by the National Natural Science Foundation of China(Nos.21866022,21567018)
the Inner Mongolia Natural Science Foundation,China(Nos.2017MS0214,2013MS0203)
the Inner Mongolia Graduate Research Innovation Project,China(No.11200-12110201)
the Project of the Inner Mongolia Key Laboratory of Environmental Pollution Control and Waste Resource Recycle,China and the Project of the Inner Mongolia Engineering Research Center of Coal Chemical Wastewater Treatment&Resourcelization,China.
