A series of CeO2‐MnOx‐Al2O3 mixed oxide catalysts （Ce：Mn：Al mole ratio=6：4：x, x=0.25, 0.5, 1, 2） were prepared by a simple one‐step inverse co‐precipitation method to investigate the influence of the incorpo...A series of CeO2‐MnOx‐Al2O3 mixed oxide catalysts （Ce：Mn：Al mole ratio=6：4：x, x=0.25, 0.5, 1, 2） were prepared by a simple one‐step inverse co‐precipitation method to investigate the influence of the incorporation of Al3＋ into CeO2‐MnOx mixed oxides. CeO2‐MnOx, CeO2‐Al2O3, and MnOx‐Al2O3 mixed oxides, and CeO2 were prepared by the same method for comparison. The samples were characterized by XRD, Raman, N2 physisorption, H2‐TPR, XPS, and in situ DRIFTS. The catalytic re‐duction of NO by CO was chosen as a model reaction to evaluate the catalytic performance. The incorporation of a small amount of Al3＋into CeO2‐MnOx mixed oxides resulted in a decrease of crys‐tallite size, with the increase of the BET specific surface area and pore volume, as well as the in‐crease of Ce3＋and Mn4＋. The former benefits good contact between catalyst and reactants, and the latter promotes the adsorption of CO and the desorption, conversion and dissociation of adsorbed NO. All these enhanced the catalytic performance for the NO＋CO model reaction. A reaction mecha‐nism was proposed to explain the excellent catalytic performance of CeO2‐MnOx‐Al2O3 catalysts for NO reduction by CO.展开更多
The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and catalytic activity tests. Acco...The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n（Ce）：n（Ti） is 5：5 or greater, and the most suitable n（Ce）：n（Ti） isdetermined as 7：3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 （n（Ce）：n（Ti）=7：3） without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2＋CO reaction show that CeO2 is the active component that offers the redox couple Ce4＋/Ce3＋ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance.展开更多
CeTiOx and CeZrTiOx catalysts were prepared by a coprecipitation method and used for selective catalytic reduction of NOx by NH3 （NH3‐SCR）. Various amounts of KNO3 were impregnated on the catalyst surface to invest...CeTiOx and CeZrTiOx catalysts were prepared by a coprecipitation method and used for selective catalytic reduction of NOx by NH3 （NH3‐SCR）. Various amounts of KNO3 were impregnated on the catalyst surface to investigate the effects of Zr addition on the K＋‐poisoning resistance of the CeTiOx catalyst. The NH3‐SCR performance of the catalysts showed that the NOx removal activity of the Zr‐modified catalyst after poisoning was better than that of the CeTiOx catalyst. Brunau‐er‐Emmett‐Teller data indicated that the Zr‐containing catalyst had a larger specific surface area and pore volume both before and after K＋poisoning. X‐ray diffraction, Raman spectroscopy, and transmission electron microscopy showed that Zr doping inhibited anatase TiO2 crystal grain growth, i.e., the molten salt flux effect caused by the loaded KNO3 was inhibited. The Ce 3d X‐ray photoelectron spectra showed that the Ce3＋/Ce4＋ratio of CeZrTiOx decreased more slowly than that of CeTiOx with increasing K＋loading, indicating that Zr addition preserved more crystal defects and oxygen vacancies; this improved the catalytic performance. The acidity was a key factor in the NH3‐SCR performance; the temperature‐programmed desorption of NH3 results showed that Zr doping inhibited the decrease in the surface acidity. The results suggest that Zr improved the K＋‐poisoning resistance of the CeTiOx catalyst.展开更多
A series of K-doped Mn0.5Ce0.5Oδ （K-MCO） catalysts with three-dimensionally ordered macroporous （3DOM） structure and different K loadings were successfully synthesized using simple methods. These catalysts exhibi...A series of K-doped Mn0.5Ce0.5Oδ （K-MCO） catalysts with three-dimensionally ordered macroporous （3DOM） structure and different K loadings were successfully synthesized using simple methods. These catalysts exhibited well-defined 3DOM nanostructure, which consisted of extensive interconnecting networks of spherical voids. The effects of the calcination temperature and calcination time on the morphological characteristics and crystalline forms of the catalysts were systematically studied. The catalysts showed high catalytic activity for the combustion of soot. 3DOM 20% K-MCO-4h catalyst, in particular, showed the highest catalytic activity of all of the catalysts studied （e.g., Ts0 = 331 ~C and Smco2 = 95.3%）. The occurrence of structural and synergistic effects among the K, Mn, and Ce atoms in the catalysts was favorable for enhancing their catalytic activity towards the combustion of diesel soot. Furthermore, the temperatures required for the complete combustion of the soot （〈400 ℃） were well within the exhaust temperature range （175-400 ℃）, which means that the accumulated soot can be removed under the conditions of the diesel exhaust gas. These catalysts could therefore be used in numerous practical applications because they are easy to synthesize, exhibit high catalytic activity, and can be made from low cost materials.展开更多
基金supported by the National Natural Science Foundation of China (21507130)the Open Project Program of Chongqing Key Laboratory of Environmental Materials and Remediation Technology from Chongqing University of Arts and Sciences (CEK1405)+3 种基金the Open Project Program of Beijing National Laboratory for Molecular Sciences (20140142)the Open Project Program of Jiangsu Key Laboratory of Vehicle Emissions Control (OVEC001)the Open Project Program of Chongqing Key Laboratory of Catalysis and Functional Organic Molecules from Chongqing Technology and Business University (1456029)the Chongqing Science & Technology Commission (cstc2014pt-gc20002)~~
文摘A series of CeO2‐MnOx‐Al2O3 mixed oxide catalysts （Ce：Mn：Al mole ratio=6：4：x, x=0.25, 0.5, 1, 2） were prepared by a simple one‐step inverse co‐precipitation method to investigate the influence of the incorporation of Al3＋ into CeO2‐MnOx mixed oxides. CeO2‐MnOx, CeO2‐Al2O3, and MnOx‐Al2O3 mixed oxides, and CeO2 were prepared by the same method for comparison. The samples were characterized by XRD, Raman, N2 physisorption, H2‐TPR, XPS, and in situ DRIFTS. The catalytic re‐duction of NO by CO was chosen as a model reaction to evaluate the catalytic performance. The incorporation of a small amount of Al3＋into CeO2‐MnOx mixed oxides resulted in a decrease of crys‐tallite size, with the increase of the BET specific surface area and pore volume, as well as the in‐crease of Ce3＋and Mn4＋. The former benefits good contact between catalyst and reactants, and the latter promotes the adsorption of CO and the desorption, conversion and dissociation of adsorbed NO. All these enhanced the catalytic performance for the NO＋CO model reaction. A reaction mecha‐nism was proposed to explain the excellent catalytic performance of CeO2‐MnOx‐Al2O3 catalysts for NO reduction by CO.
文摘The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n（Ce）：n（Ti） is 5：5 or greater, and the most suitable n（Ce）：n（Ti） isdetermined as 7：3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 （n（Ce）：n（Ti）=7：3） without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2＋CO reaction show that CeO2 is the active component that offers the redox couple Ce4＋/Ce3＋ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance.
基金supported by the Major Research Program of Sichuan Province Science and Technology Department (2012FZ0008)the National Natural Science Foundation of China (21173153)+1 种基金the National High Technology Research and Development Program of China (863 Program,2013AA065304)the Sichuan University Research Foundation for Young Teachers (2015SCU11056)~~
文摘CeTiOx and CeZrTiOx catalysts were prepared by a coprecipitation method and used for selective catalytic reduction of NOx by NH3 （NH3‐SCR）. Various amounts of KNO3 were impregnated on the catalyst surface to investigate the effects of Zr addition on the K＋‐poisoning resistance of the CeTiOx catalyst. The NH3‐SCR performance of the catalysts showed that the NOx removal activity of the Zr‐modified catalyst after poisoning was better than that of the CeTiOx catalyst. Brunau‐er‐Emmett‐Teller data indicated that the Zr‐containing catalyst had a larger specific surface area and pore volume both before and after K＋poisoning. X‐ray diffraction, Raman spectroscopy, and transmission electron microscopy showed that Zr doping inhibited anatase TiO2 crystal grain growth, i.e., the molten salt flux effect caused by the loaded KNO3 was inhibited. The Ce 3d X‐ray photoelectron spectra showed that the Ce3＋/Ce4＋ratio of CeZrTiOx decreased more slowly than that of CeTiOx with increasing K＋loading, indicating that Zr addition preserved more crystal defects and oxygen vacancies; this improved the catalytic performance. The acidity was a key factor in the NH3‐SCR performance; the temperature‐programmed desorption of NH3 results showed that Zr doping inhibited the decrease in the surface acidity. The results suggest that Zr improved the K＋‐poisoning resistance of the CeTiOx catalyst.
基金supported by the National Natural Science Foundation of China(21177160,21303263,21477164)Beijing Nova Program(Z141109001814072)+1 种基金Specialized Research Fund for the Doctoral Program of High Education of China(20130007120011)the Science Foundation of China University of Petroleum-Beijing(2462013YJRC13,2462013BJRC003)~~
文摘A series of K-doped Mn0.5Ce0.5Oδ （K-MCO） catalysts with three-dimensionally ordered macroporous （3DOM） structure and different K loadings were successfully synthesized using simple methods. These catalysts exhibited well-defined 3DOM nanostructure, which consisted of extensive interconnecting networks of spherical voids. The effects of the calcination temperature and calcination time on the morphological characteristics and crystalline forms of the catalysts were systematically studied. The catalysts showed high catalytic activity for the combustion of soot. 3DOM 20% K-MCO-4h catalyst, in particular, showed the highest catalytic activity of all of the catalysts studied （e.g., Ts0 = 331 ~C and Smco2 = 95.3%）. The occurrence of structural and synergistic effects among the K, Mn, and Ce atoms in the catalysts was favorable for enhancing their catalytic activity towards the combustion of diesel soot. Furthermore, the temperatures required for the complete combustion of the soot （〈400 ℃） were well within the exhaust temperature range （175-400 ℃）, which means that the accumulated soot can be removed under the conditions of the diesel exhaust gas. These catalysts could therefore be used in numerous practical applications because they are easy to synthesize, exhibit high catalytic activity, and can be made from low cost materials.
