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
In this study,a series of Mn-Ce/Al_(2)O_(3) catalysts was prepared by different methods of depositionprecipitation(MnCeAl-DP),impregnation(MnCeAl-IM) and citric acid(MnCeAl-CA),and the distinct effect of preparation m...In this study,a series of Mn-Ce/Al_(2)O_(3) catalysts was prepared by different methods of depositionprecipitation(MnCeAl-DP),impregnation(MnCeAl-IM) and citric acid(MnCeAl-CA),and the distinct effect of preparation methods on NO_(x) removal performance at low temperature was explored.Results show that MnCeAl-DP exhibits not only the best activity but also the highest resistance against SO_(2)/H_(2)O.With the assistance of comprehensive characterizations from scanning electron microscopy(SEM),Brunauer-Emmett-Teller(BET),X-ray diffraction(XRD),H_(2)-temperature programmed reduction(H_(2)-TPR),NH_(3)-te mperature programmed deso rption(NH_(3)-TPD),and X-ray photoelectron spectroscopy(XPS),it is revealed that the MnCeAl-DP sample owns admired features of large surface area and pore volume,enriched Mn^(4+) and chemisorbed oxygen species originating from enhanced interaction between MnO_x and CeO_(2),as well as improved adsorption capacity to NH_(3) and NO.All these factors contribute to activity enhancement.Further in-situ DRIFTS studies reveal that the improvement of NH_(3)-SCR performance over MnCeAI-DP is related to the formation of abundant nitrate species,which is beneficial to the "NH_(4)NO_(3)" reaction pathway and thus enhances low-temperature activity.展开更多
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.
基金Project supported by the National Natural Science Foundation of China (22272077,22276097,21976081)Major Scientific and Technological Project of Bingtuan (2018AA002)。
文摘In this study,a series of Mn-Ce/Al_(2)O_(3) catalysts was prepared by different methods of depositionprecipitation(MnCeAl-DP),impregnation(MnCeAl-IM) and citric acid(MnCeAl-CA),and the distinct effect of preparation methods on NO_(x) removal performance at low temperature was explored.Results show that MnCeAl-DP exhibits not only the best activity but also the highest resistance against SO_(2)/H_(2)O.With the assistance of comprehensive characterizations from scanning electron microscopy(SEM),Brunauer-Emmett-Teller(BET),X-ray diffraction(XRD),H_(2)-temperature programmed reduction(H_(2)-TPR),NH_(3)-te mperature programmed deso rption(NH_(3)-TPD),and X-ray photoelectron spectroscopy(XPS),it is revealed that the MnCeAl-DP sample owns admired features of large surface area and pore volume,enriched Mn^(4+) and chemisorbed oxygen species originating from enhanced interaction between MnO_x and CeO_(2),as well as improved adsorption capacity to NH_(3) and NO.All these factors contribute to activity enhancement.Further in-situ DRIFTS studies reveal that the improvement of NH_(3)-SCR performance over MnCeAI-DP is related to the formation of abundant nitrate species,which is beneficial to the "NH_(4)NO_(3)" reaction pathway and thus enhances low-temperature activity.
