Composite supports Zr0.5Al0.5O1.75 modified by metal oxides,such as La2O3,ZnO,Y2O3 or BaO,were prepared by co-precipitation method,and palladium catalysts supported on the modified composite supports were prepared by impregnation method.Their properties were characterized by X-ray diffraction(XRD),NH3 temperature-programmed desorption(NH3-TPD),H2 temperature-programmed reduction(H2-TPR),N2 adsorption/desorption,and CO-chemisorption.The catalytic activity and the resistance to water poisoning of the prepared Pd catalysts were tested in a simulated exhaust gas from lean-burn natural gas vehicles with and without water vapor.The results demonstrated that the modified supports had an apparent effect on the performance of Pd catalysts,compared with the Pd catalyst supported on the unmodified ZrAl.The addition of ZnO or Y2O3 promoted the conversion of CH4.In the absence of water vapor,Pd/ZnZrAl exhibited the best activity for CH4 conversion with the light-off temperature(T50) of 275℃ and the complete conversion temperature(T90) of 314℃,respectively.However,in the presence of water vapor,Pd/YZrAl was the best one over which the light-off temperature(T50) of methane was 339℃ and the complete conversion temperature(T90) was 371℃.These results indicated that Pd catalyst supported on the modified composite ZrAl support showed excellent catalytic activity at low temperature and high resistance to H2O poisoning for the exhaust purification of lean-burn natural gas vehicles.
A series of CexZr1-xO2(0 B x B 1)with different molar ratios of Ce/Zr were syhthesized via coprecipitation method,and Fe2O3-WO3/CexZr1-xO2monolithic catalysts were prepared for selective catalytic reduction of nitrogen oxides by ammonia(NH3-SCR).The structural properties and redox behavior of the catalysts were comprehensively characterized by N2physisorption,X-ray diffraction(XRD),X-ray photoelectron spectra(XPS),H2-temperature programmed reduction(H2-TPR)and activity measurement for NH3-SCR.The results showed that the NH3-SCR activities of the catalysts were gradually enhanced by increasing the molar ratios of Ce/Zr,especially the lowtemperature catalytic activity and the reaction temperature window.Fe2O3-WO3/Ce0.68Zr0.32O2monolithic catalyst presented the best NH3-SCR activity among the investigated catalysts,more than 90%NOxcould be removed in the temperature range of 247–454°C on the catalyst under the gas hourly space velocities of 30,000 h-1.And it always held more than 99%N2selectivity and less than 20 ppm(1 ppm=10-6L/L)N2O generation concentration between 200 and500°C,the catalyst also displayed its strong resistance of H2O and SO2.Good textural and structural properties,more surface Fe,Ce and active oxygen were together contributed to the excellent NH3-SCR performance of Fe2O3-WO3/Ce0.68Zr0.32O2catalyst.
