A nanoporous MoO3/ZrO2 mixed oxide was hydrothermally synthesized by hydrolyzing zirconium isopropoxide in the presence of a cationic surfactant, eetyltrimethylammonium bromide(CTAB). The crystal structure and the a...A nanoporous MoO3/ZrO2 mixed oxide was hydrothermally synthesized by hydrolyzing zirconium isopropoxide in the presence of a cationic surfactant, eetyltrimethylammonium bromide(CTAB). The crystal structure and the acidity of the obtained nanoporous MoO3/ZrO2 mixed oxide were determined by means of XRD, N2 adsorption-desorption and NH3-TPD, respectively. The isobutane/butene alkylation over the MoO3/ZrO2 catalyst was carried out in a fixed bed reactor. The results reveal that ZrO2 in MoO3/ZrO2 exists mainly in the tetragonal phase, and the catalyst samples possess large specific surface areas as well as moderate acidity for isobutane/butene alkylation. Compared with samples prepared by impregnation and sol-gel processes, MoO3/ZrO2 mixed oxide samples prepared in this work have a better catalytic activity.展开更多
A solid superacid catalyst Pt-SO42-/ZrO2-A12O3 for n-pentane isomerization, was prepared by incipient-wetness impregnation. Preparetion conditions, namely, calcination temperature, concentration of sulfuric acid solut...A solid superacid catalyst Pt-SO42-/ZrO2-A12O3 for n-pentane isomerization, was prepared by incipient-wetness impregnation. Preparetion conditions, namely, calcination temperature, concentration of sulfuric acid solution used in impregnation and Al2O3 concentration, were varied to investigate the effects on catalytic performance of Pt-SO42-/ZrO2-A12O3. The results showed that the PtSZA catalyst exhibited excellent catalytic performance for n-pentane isomerization. Under optimized preparation conditions of calcination temperature of 650°C, reaction time for 3 h, concentration of sulfuric acid solution for 0.5 mol/L, 30% of Al2O3 concentration and 0.3% of Pt concentration, the n-pentane conversion and isopentane selectivity of Pt-SO42-/ZrO2-A12O3 could reach up to 62.17% and 91.60%, respectively.展开更多
A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐W...A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐WO3/TiO2 catalyst.The physicochemical properties were investigated by using XRD,BET,NH3‐TPD,H2‐TPR,and XPS,and the catalytic performance and K‐poisoning resistance were evaluated via a NH3‐SCR model reaction.Ce^4+and Zr^4+co‐doping were found to enhance the conversion of NOx,and exhibit the best K‐poisoning resistance owing to the largest BET‐specific surface area,pore volume,and total acid site concentration,as well as the minimal effects on the surface acidity and redox ability from K poisoning.The V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst also presents outstanding H2O+SO2 tolerance.Finally,the in situ DRIFTS reveals that the NH3‐SCR reaction over the V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst follows an L‐H mechanism,and that K poisoning does not change the reaction mechanism.展开更多
The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/...The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi(CN/BMO/Bi)hollow microsphere was successfully fabricated through solvothermal and in situ reduction methods.The results revealed that the optimal ternary 0.4 CN/BMO/9 Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B(RhB)degradation with nine times that of pure BMO.The DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4 CN/BMO/9 Bi is a z-scheme structure.Quenching experiments also provided solid evidence that the·O^2-(at-0.33 eV)is the main species during dye degradation,and the conduction band of g-C3N4 is only the reaction site,demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2 MoO 6/Bi is through an indirect z-scheme structure.Thus,the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping,resulting in better optical absorption ability and a lower combination rate of photogenerated charge carriers.The findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.展开更多
Zirconium hydroxide synthesized by sol-gel was impregnated with an aqueous solution of ammonium heptamolybdate in order to obtain 15 wt% of MoO3 on ZrO2. Pure and modified hydroxides were calcined at 400, 500, and 600...Zirconium hydroxide synthesized by sol-gel was impregnated with an aqueous solution of ammonium heptamolybdate in order to obtain 15 wt% of MoO3 on ZrO2. Pure and modified hydroxides were calcined at 400, 500, and 600 ℃. In order to evaluate the catalytic activity for n-hexane isomerization, the materials were impregnated with 0.5 wt% of platinum and treated at 400 ℃. For pure ZrO2 it was observed that the surface area decreases from 144 to 18 m2/g when the calcination temperature increases from 400 to 600℃ The addition of Mo to zirconia increases the specific surface area (238-130 m^2/g) in samples treated at the same temperatures. Pure zirconia transformed from tetragonal to monoclinic phase when calcined between 400 and 600 ℃. However, this transformation did not occur in the ZrO2-MoO3 supports. The n-butylamine results showed that all the ZrO2-MoO3 supports presented a higher acidity (〉 255 mV) than that corresponding to pure ZrO2 (- 48 mV), which presented only weakly acidic sites. Pt/ZrO2-MoO3 calcined at 600 ℃ proved to be the best catalyst for n-hexane isomerization, presenting a high selectivity to isomerization products (82%) at high conversion (72%).展开更多
摘要A nanoporous MoO3/ZrO2 mixed oxide was hydrothermally synthesized by hydrolyzing zirconium isopropoxide in the presence of a cationic surfactant, eetyltrimethylammonium bromide(CTAB). The crystal structure and the acidity of the obtained nanoporous MoO3/ZrO2 mixed oxide were determined by means of XRD, N2 adsorption-desorption and NH3-TPD, respectively. The isobutane/butene alkylation over the MoO3/ZrO2 catalyst was carried out in a fixed bed reactor. The results reveal that ZrO2 in MoO3/ZrO2 exists mainly in the tetragonal phase, and the catalyst samples possess large specific surface areas as well as moderate acidity for isobutane/butene alkylation. Compared with samples prepared by impregnation and sol-gel processes, MoO3/ZrO2 mixed oxide samples prepared in this work have a better catalytic activity.
摘要A solid superacid catalyst Pt-SO42-/ZrO2-A12O3 for n-pentane isomerization, was prepared by incipient-wetness impregnation. Preparetion conditions, namely, calcination temperature, concentration of sulfuric acid solution used in impregnation and Al2O3 concentration, were varied to investigate the effects on catalytic performance of Pt-SO42-/ZrO2-A12O3. The results showed that the PtSZA catalyst exhibited excellent catalytic performance for n-pentane isomerization. Under optimized preparation conditions of calcination temperature of 650°C, reaction time for 3 h, concentration of sulfuric acid solution for 0.5 mol/L, 30% of Al2O3 concentration and 0.3% of Pt concentration, the n-pentane conversion and isopentane selectivity of Pt-SO42-/ZrO2-A12O3 could reach up to 62.17% and 91.60%, respectively.
基金supported by the National Natural Science Foundation of China(21876168,21507130)the Key Projects for Common Key Technology Innovation in Key Industries in Chongqing(cstc2016zdcy-ztzx0020-01)+2 种基金the Chongqing Science&Technology Commission(cstc2016jcyjA0070,cstckjcxljrc13)the Open Project Program of Chongqing Key Laboratory of Catalysis and Functional Organic Molecules from Chongqing Technology and Business University(1456029)the Graduate Innovation Project of Chongqing Technology and Business University(yjscxx201803-028-22)~~
摘要A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐WO3/TiO2 catalyst.The physicochemical properties were investigated by using XRD,BET,NH3‐TPD,H2‐TPR,and XPS,and the catalytic performance and K‐poisoning resistance were evaluated via a NH3‐SCR model reaction.Ce^4+and Zr^4+co‐doping were found to enhance the conversion of NOx,and exhibit the best K‐poisoning resistance owing to the largest BET‐specific surface area,pore volume,and total acid site concentration,as well as the minimal effects on the surface acidity and redox ability from K poisoning.The V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst also presents outstanding H2O+SO2 tolerance.Finally,the in situ DRIFTS reveals that the NH3‐SCR reaction over the V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst follows an L‐H mechanism,and that K poisoning does not change the reaction mechanism.
基金financially supported by the Science Foundation of China University of Petroleum,Beijing(2462017YJRC048,2462018BJC005)the National Natural Science Foundation of China(51802351)~~
摘要The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi(CN/BMO/Bi)hollow microsphere was successfully fabricated through solvothermal and in situ reduction methods.The results revealed that the optimal ternary 0.4 CN/BMO/9 Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B(RhB)degradation with nine times that of pure BMO.The DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4 CN/BMO/9 Bi is a z-scheme structure.Quenching experiments also provided solid evidence that the·O^2-(at-0.33 eV)is the main species during dye degradation,and the conduction band of g-C3N4 is only the reaction site,demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2 MoO 6/Bi is through an indirect z-scheme structure.Thus,the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping,resulting in better optical absorption ability and a lower combination rate of photogenerated charge carriers.The findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.
摘要Zirconium hydroxide synthesized by sol-gel was impregnated with an aqueous solution of ammonium heptamolybdate in order to obtain 15 wt% of MoO3 on ZrO2. Pure and modified hydroxides were calcined at 400, 500, and 600 ℃. In order to evaluate the catalytic activity for n-hexane isomerization, the materials were impregnated with 0.5 wt% of platinum and treated at 400 ℃. For pure ZrO2 it was observed that the surface area decreases from 144 to 18 m2/g when the calcination temperature increases from 400 to 600℃ The addition of Mo to zirconia increases the specific surface area (238-130 m^2/g) in samples treated at the same temperatures. Pure zirconia transformed from tetragonal to monoclinic phase when calcined between 400 and 600 ℃. However, this transformation did not occur in the ZrO2-MoO3 supports. The n-butylamine results showed that all the ZrO2-MoO3 supports presented a higher acidity (〉 255 mV) than that corresponding to pure ZrO2 (- 48 mV), which presented only weakly acidic sites. Pt/ZrO2-MoO3 calcined at 600 ℃ proved to be the best catalyst for n-hexane isomerization, presenting a high selectivity to isomerization products (82%) at high conversion (72%).