The catalysts of iron-doped Mn-Ce/TiO2 （Fe-Mn-Ce/TiO2） prepared by sol-gel method were investigated for low temperature selective catalytic reduction （SCR） of NO with NH3. It was found that the NO conversion over ...The catalysts of iron-doped Mn-Ce/TiO2 （Fe-Mn-Ce/TiO2） prepared by sol-gel method were investigated for low temperature selective catalytic reduction （SCR） of NO with NH3. It was found that the NO conversion over Fe-Mn-Ce/TiO2 was obviously improved after iron doping compared with that over Mn-Ce/TiO2. Fe-Mn-Ce/TiO2 with the molar ratio of Fe/Ti = 0.1 exhibited the highest activity. The results showed that 96.8% NO conversion was obtained over Fe（0.1）-Mn-Ce/TiO2 at 180~C at a space velocity of 50,000 hr-1. Fe-Mn-Ce/TiO2 exhibited much higher resistance to H2O and SO2 than that of Mn-Ce/TiO2. The properties of the catalysts were characterized using X-ray diffraction （XRD）, N2 adsorption, temperature programmed desorption （NH3-TPD and NOx-TPD）, and X- ray photoelectron spectroscopy （XPS） techniques. BET, NH3-TPD and NOx-TPD results showed that the specific surface area and NH3 and NOx adsorption capacity of the catalysts increased with iron doping. It was known from XPS analysis that iron valence state on the surface of the catalysts were in Fe^3＋ state. The doping of iron enhanced the dispersion and oxidation state of Mn and Ce on the surface of the catalysts. The oxygen concentrations on the surface of the catalysts were found to increase after iron doping. Fe-Mn-Ce/TiO2 represented a promising catalyst for low temperature SCR of NO with NH3 in the presence of H20 and SO2.展开更多
SO2 poisoning and regeneration of Mn-Ce/TiO2 catalyst prepared by a novel co-precipitation method for low temperature selective catalytic reduction （SCR） of NOx with ammonia were investigated in this study. When 700...SO2 poisoning and regeneration of Mn-Ce/TiO2 catalyst prepared by a novel co-precipitation method for low temperature selective catalytic reduction （SCR） of NOx with ammonia were investigated in this study. When 700 ppm SO2 was fed in, the Mn-Ce/TiO2 catalyst had good resistance to SO2, but the deactivation of Mn-Ce/TiO2 poisoned by SO2 still occurred. The NO conversion of Mn-Ce/TiO2 （the molar ra-tio of Ce to Ti is 0.075） catalyst decreased from 92.5% to 34.6% in 13 h. Characterizations of fresh and SO2-poisoned Mn-Ce/TiO2 catalysts were carried out by Brunauer-Emmett-Teller method （BET）, ion chromatography （IC）, X-ray photoelectron spectroscopy （XPS）, and X-ray diffraction （XRD）. The characterized results indicated that the deposition of sulfates and nitrates on the surface made the catalyst deactivated. Water washing, thermal regeneration and reductive regeneration were used to regenerate the deactivated Mn-Ce/TiO2. And water washing showed best performance on the regeneration of poisoned catalysts, especially with ultrasonic vibration. The Mn-Ce/TiO2 catalyst showed high stability under a series of deactivation-regeneration experiments for ten cycles.展开更多
基金supported by the National Natural Science Foundation of China (No. 90610018,50976050)the New Century Excellent Talents in University (No. NCET-07-0457)the National Key Technologies R&D Program of Tianjin (No. 09ZCKFSH01900)
文摘The catalysts of iron-doped Mn-Ce/TiO2 （Fe-Mn-Ce/TiO2） prepared by sol-gel method were investigated for low temperature selective catalytic reduction （SCR） of NO with NH3. It was found that the NO conversion over Fe-Mn-Ce/TiO2 was obviously improved after iron doping compared with that over Mn-Ce/TiO2. Fe-Mn-Ce/TiO2 with the molar ratio of Fe/Ti = 0.1 exhibited the highest activity. The results showed that 96.8% NO conversion was obtained over Fe（0.1）-Mn-Ce/TiO2 at 180~C at a space velocity of 50,000 hr-1. Fe-Mn-Ce/TiO2 exhibited much higher resistance to H2O and SO2 than that of Mn-Ce/TiO2. The properties of the catalysts were characterized using X-ray diffraction （XRD）, N2 adsorption, temperature programmed desorption （NH3-TPD and NOx-TPD）, and X- ray photoelectron spectroscopy （XPS） techniques. BET, NH3-TPD and NOx-TPD results showed that the specific surface area and NH3 and NOx adsorption capacity of the catalysts increased with iron doping. It was known from XPS analysis that iron valence state on the surface of the catalysts were in Fe^3＋ state. The doping of iron enhanced the dispersion and oxidation state of Mn and Ce on the surface of the catalysts. The oxygen concentrations on the surface of the catalysts were found to increase after iron doping. Fe-Mn-Ce/TiO2 represented a promising catalyst for low temperature SCR of NO with NH3 in the presence of H20 and SO2.
基金financially supported by the Research Project of China Guodian Corporation (No.D11T22)
文摘SO2 poisoning and regeneration of Mn-Ce/TiO2 catalyst prepared by a novel co-precipitation method for low temperature selective catalytic reduction （SCR） of NOx with ammonia were investigated in this study. When 700 ppm SO2 was fed in, the Mn-Ce/TiO2 catalyst had good resistance to SO2, but the deactivation of Mn-Ce/TiO2 poisoned by SO2 still occurred. The NO conversion of Mn-Ce/TiO2 （the molar ra-tio of Ce to Ti is 0.075） catalyst decreased from 92.5% to 34.6% in 13 h. Characterizations of fresh and SO2-poisoned Mn-Ce/TiO2 catalysts were carried out by Brunauer-Emmett-Teller method （BET）, ion chromatography （IC）, X-ray photoelectron spectroscopy （XPS）, and X-ray diffraction （XRD）. The characterized results indicated that the deposition of sulfates and nitrates on the surface made the catalyst deactivated. Water washing, thermal regeneration and reductive regeneration were used to regenerate the deactivated Mn-Ce/TiO2. And water washing showed best performance on the regeneration of poisoned catalysts, especially with ultrasonic vibration. The Mn-Ce/TiO2 catalyst showed high stability under a series of deactivation-regeneration experiments for ten cycles.
