摘要
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.
A series of CexZrl_xO2 （0 ≤ x ≤ 1） with dif- ferent molar ratios of Ce/Zr were syhthesized via coprecip- itation method, and Fe2O3-WO3/CexZrl-xO2 monolithic catalysts were prepared, for selective catalytic reduction of nitrogen oxides by ammonia （NH3-SCR）. The structural properties and redox behavior of the catalysts were com- prehensively characterized by N2 physisorption, 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 low- temperature catalytic activity and the reaction temperature window. Fe2O3-WO3/Ceo.68Zro.3202 monolithic catalyst presented the best NH3-SCR activity among the investigated catalysts, more than 90 % NOx could be removed in the temperature range of 247-454 ℃ on the catalyst under the gas hourly space velocities of 30,000 h- 1. And it always held more than 99 % N2 selectivity and less than 20 ppm （1 ppm =10-6 L/L ） N20 generation concentration between 200 and 500 ℃, the catalyst also displayed its strong resistance of H20 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/ Ce0.68Zr0.32O2 catalyst.
基金
supported by the National Natural Science Foundation of China(21173153)
the Project from Sichuan Provincial Environment Office of China(2011HB002)
the National High Technology Research and Development Program of China(2013AA065304)
