Sm-doped Fe_(2)O_(3)catalysts,with a homogeneous distribution of Sm in Fe_(2)O_(3)nanoparticles,were synthesized using a citric acid-assisted sol-gel method.Kinetic studies show that the reaction rate for NO_(x)reduct...Sm-doped Fe_(2)O_(3)catalysts,with a homogeneous distribution of Sm in Fe_(2)O_(3)nanoparticles,were synthesized using a citric acid-assisted sol-gel method.Kinetic studies show that the reaction rate for NO_(x)reduction using the optimal catalyst(0.06 mol%doping of Sm in Fe_(2)O_(3))was nearly 11 times higher than that for pure Fe_(2)O_(3),when calculated based on specific surface area.Furthermore,the Fe_(0.94)Sm_(0.06)O_(x)catalyst maintains>83%NO_(x)conversion for 168 h at a high space velocity in the presence of SO_(2)and H_(2)O at 250℃.A substantial amount of surface-adsorbed oxygen was generated on the surface of Fe_(0.94)Sm_(0.06)O_(x),which promoted NO oxidation and the subsequent fast reaction between NO_(x)and NH_(3).The adsorption and activation of NH_(3)was also enhanced by Sm doping.In addition,Sm doping facilitated the decomposition of NH_(4)HSO_(4)on the surface of Fe_(0.94)Sm_(0.06)O_(x),resulting in its high activity and stability in the presence of SO_(2)+H_(2)O.展开更多
NH_(3)-SCR is an effective mean of NOxremoval in the non-electric industry, however, the high activation temperature and poor H_(2)O resistance of SCR catalysts posed a barrier to its application. In this work, a seri...NH_(3)-SCR is an effective mean of NOxremoval in the non-electric industry, however, the high activation temperature and poor H_(2)O resistance of SCR catalysts posed a barrier to its application. In this work, a series of three-dimensionally ordered macroporous(3DOM) catalysts were synthesized via a colloidal crystal template(CCT) method, and various characterizations were carried out to explore the physicochemical property of catalysts. The experiment results reveal that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst presents the excellent low-temperature catalytic activity of nearly 100% at 100℃. Furthermore, the enhanced H_(2)O resistance is achieved, certified by the unaffected NO remove at 150℃ in the participation of 15 vol% H_(2)O. The characterizations results exhibit that the improved dispersion of the active component and enhanced redox ability are conducive to the low-temperature catalytic activity. N_(2) adsorption and desorption experiments indicate that catalyst with 3DOM support possesses a larger pore diameter and specific surface area, which may weaken the condensation of H_(2)O in the microporosity of catalysts and improved the H_(2)O resistance of the catalyst. In situ DRIFTS results manifest that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst could not only absorb more NH_(3) and generate more surface-active sites, but inhibit the competitive adsorption between H_(2)O and SCR reactants.展开更多
Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts...Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts(denoted as xSFeCeVWTi) significantly enhances its alkali resistance with K element as a representative.A series of xSFeCeVWTi catalysts was synthesized by wet impregnation with designed 0.05Fe/V, 1.5Ce/V and different S/V molar ratios x.The NO_(x) conversion and K resistance of xSFeCeVWTi catalysts increase with the increase of loading amounts of sulfates but no longer further increase as the sulfates load is excessive to block the pores of catalysts and hinder the adsorption of reactants.The optimal modified catalyst in about 2.2S/V actual loading ratio,corresponding to 10.5SFeCeVWTi sample,shows over 99.0%NO_(x) conversion and N_(2) selectivity at 300-400℃ after K-poisoning.The interaction between Fe,Ce and V improves its redox ability but slightly weakens surface acidity,while the proper amount of sulfate species enriches surface Br?nsted acid sites but attenuates its redox capability.However,a balance of redox capacity and surface acidity,caused by Fe,Ce and sulfate co-modification,contributes to the excellent K resistance of 10.5SFeCeVWTi catalyst.Finally,the change of physicochemical properties influences the reaction mechanism which follows the Eley-Rideal mechanism on 10.SSFeCeVWTi catalyst.These results show that the co-modification with Fe,Ce and sulfates is a good way to improve the alkali tolerance of V_(2)O_(5)-WO_(3)/TiO_(2) catalyst in industrial applications.展开更多
文摘Sm-doped Fe_(2)O_(3)catalysts,with a homogeneous distribution of Sm in Fe_(2)O_(3)nanoparticles,were synthesized using a citric acid-assisted sol-gel method.Kinetic studies show that the reaction rate for NO_(x)reduction using the optimal catalyst(0.06 mol%doping of Sm in Fe_(2)O_(3))was nearly 11 times higher than that for pure Fe_(2)O_(3),when calculated based on specific surface area.Furthermore,the Fe_(0.94)Sm_(0.06)O_(x)catalyst maintains>83%NO_(x)conversion for 168 h at a high space velocity in the presence of SO_(2)and H_(2)O at 250℃.A substantial amount of surface-adsorbed oxygen was generated on the surface of Fe_(0.94)Sm_(0.06)O_(x),which promoted NO oxidation and the subsequent fast reaction between NO_(x)and NH_(3).The adsorption and activation of NH_(3)was also enhanced by Sm doping.In addition,Sm doping facilitated the decomposition of NH_(4)HSO_(4)on the surface of Fe_(0.94)Sm_(0.06)O_(x),resulting in its high activity and stability in the presence of SO_(2)+H_(2)O.
基金Project supported by National Key Research and Development Program of China(2021YFB3500601)。
文摘NH_(3)-SCR is an effective mean of NOxremoval in the non-electric industry, however, the high activation temperature and poor H_(2)O resistance of SCR catalysts posed a barrier to its application. In this work, a series of three-dimensionally ordered macroporous(3DOM) catalysts were synthesized via a colloidal crystal template(CCT) method, and various characterizations were carried out to explore the physicochemical property of catalysts. The experiment results reveal that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst presents the excellent low-temperature catalytic activity of nearly 100% at 100℃. Furthermore, the enhanced H_(2)O resistance is achieved, certified by the unaffected NO remove at 150℃ in the participation of 15 vol% H_(2)O. The characterizations results exhibit that the improved dispersion of the active component and enhanced redox ability are conducive to the low-temperature catalytic activity. N_(2) adsorption and desorption experiments indicate that catalyst with 3DOM support possesses a larger pore diameter and specific surface area, which may weaken the condensation of H_(2)O in the microporosity of catalysts and improved the H_(2)O resistance of the catalyst. In situ DRIFTS results manifest that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst could not only absorb more NH_(3) and generate more surface-active sites, but inhibit the competitive adsorption between H_(2)O and SCR reactants.
基金Project supported by Fujian Provincial Department of Science and Technology,China (2020Y0085)Youth Innovation Promotion Association,Chinese Academy of Sciences (2020309)the Cultivating Project of Strategic Priority Research Program of Chinese Academy of Sciences (XDPB1902)。
文摘Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts(denoted as xSFeCeVWTi) significantly enhances its alkali resistance with K element as a representative.A series of xSFeCeVWTi catalysts was synthesized by wet impregnation with designed 0.05Fe/V, 1.5Ce/V and different S/V molar ratios x.The NO_(x) conversion and K resistance of xSFeCeVWTi catalysts increase with the increase of loading amounts of sulfates but no longer further increase as the sulfates load is excessive to block the pores of catalysts and hinder the adsorption of reactants.The optimal modified catalyst in about 2.2S/V actual loading ratio,corresponding to 10.5SFeCeVWTi sample,shows over 99.0%NO_(x) conversion and N_(2) selectivity at 300-400℃ after K-poisoning.The interaction between Fe,Ce and V improves its redox ability but slightly weakens surface acidity,while the proper amount of sulfate species enriches surface Br?nsted acid sites but attenuates its redox capability.However,a balance of redox capacity and surface acidity,caused by Fe,Ce and sulfate co-modification,contributes to the excellent K resistance of 10.5SFeCeVWTi catalyst.Finally,the change of physicochemical properties influences the reaction mechanism which follows the Eley-Rideal mechanism on 10.SSFeCeVWTi catalyst.These results show that the co-modification with Fe,Ce and sulfates is a good way to improve the alkali tolerance of V_(2)O_(5)-WO_(3)/TiO_(2) catalyst in industrial applications.
