Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction bet...Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction between high crystallinity and high surface area,the synthesis of mesoporous SMOs heterojunctions with highly o rdered mesostructures,highly crystallized frameworks,and high surface area remains a huge challenge.In this work,we develop a novel"acid-base pair"adjusted solvent evaporation induced self-assembly(EISA)strategy to prepare highly crystallized ordered mesoporous TiO2/WO3(OM-TiO2/WO3)heterojunctions.The WCl6 and titanium isopropoxide(TIPO)are used as the precursors,respectively,which function as the"acid-base pair",enabling the coassembly with the structure directing agent(PEO-b-PS)into highly ordered meso structures.In addition,PEO-b-PS can be converted to rigid carbon which can protect the meso structures from collapse during the crystallization process.The resultant OM-TiO2/WO3 heterojunctions possess primitive cubic mesostructures,large pore size(~21.1 nm),highly crystalline frameworks and surface area(~98 m2/g).As a sensor for acetone,the obtained OM-TiO2/WO3 show excellent re sponse/recovery perfo rmance(3 s/5 s),good linear dependence,repeatability,selectivity,and long-term stability(35 days).展开更多
8wt%WO3/SiO2 metathesis （disproportionation） catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-deso...8wt%WO3/SiO2 metathesis （disproportionation） catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-desorption, scanning electron microscopy （SEM）, X-ray diffraction （XRD）, UV-visible diffuse reflectance spectroscopy （DRS） and scanning transmission electron microscopy-high-angle annular dark field （STEM HAADF）. The results of STEM HAADF showed that WO3 species were not uniformly distributed on the SiO2 support. The experimental results of 8wt%WO3/SiO2 performance in ethene/decene metathesis revealed that the catalytic effect of 8wt%WO3/SiO2 catalyst and coke formation over it were closely related to the support pore structure： The 8wt%WO3/SiO2 catalyst with a more complicated pore structure showed better catalytic performance but the coke deposition rate was also faster.展开更多
The selective catalytic reduction of NOV with NH3 (NH3-SCR) is a very effective technology to control the emission of NOA, and the thermal stability of NH3-SCR catalyst is very important for removal of NOV from diesel...The selective catalytic reduction of NOV with NH3 (NH3-SCR) is a very effective technology to control the emission of NOA, and the thermal stability of NH3-SCR catalyst is very important for removal of NOV from diesel engines. In this work, V2O5/WO3-TiO2 (VWT) and SiO2- doped V2O5/WO3-TiO2 (VWTSi10)) catalysts were prepared by impregnation method and characterized by Brunauer- Emmett-Teller (BET), X-ray diffraction (XRD), Raman, temperature programmed reduction by hydrogen (H2-TPR), X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption by ammonia (NH3- TPD). The doping of SiO2 promotes the thermal stability of V2O5/WO3-TiO? for NH3-SCR significantly. After calcination at 650 °C for 50 h, the operation window of 10% SiO2-doped V2O5/WO3-TiO2 is 220-480 °C, while the maximum NOV conversion on V2O5/WO3-TiO2 is about 77%. The presenee of SiO2 obviously blocks the transformation of TiO2 from anatase to rutile and stabilizes the dispersion of VOv and WO3 on the surface. It is available for the existence of V44 and the amount of surface acid sites increases, which inhabits the NH3 oxidation at the high temperature range and promotes NH3-SCR activity.展开更多
The effects of the initial framework SiO2/Al2O3 ratio and temperature on the structural changes of NaY zeolites during hydrothermal treatments are studied. Two samples with different framework SiO2/Al2O3 ratios are ...The effects of the initial framework SiO2/Al2O3 ratio and temperature on the structural changes of NaY zeolites during hydrothermal treatments are studied. Two samples with different framework SiO2/Al2O3 ratios are subjected to hydrothermal treatment at four different temperatures. For zeolite with a lower initial SiO2/Al2O3 ratio of 4.2, mesopores are easily formed because more framework aluminum is detached. Moreover, two kinds of mesopores are produced at a higher temperature due to the interconnection of vacancies and smaller mesopores. For zeolite with a higher initial SiO2/Al2O3 ratio of 6.0, there are less mesopores formed as compared with the lower initial SiO2/Al2O3 ratio sample, but there are some macropores formed. This may be attributed to the isolation of vacancies and the different distributions of aluminum in the crystal lattice of the zeolite. The experiment data show that NaY with the SiO2/Al2O3 ratio of 6.0 retains a high relative crystallinity during the hydrothermal treatment. This proves that a high framework SiO2/Al2O3 ratio benefits the stability of zeolite.展开更多
基金supported by the National Natural Science Foundation of China(Nos.51822202 and 51772050)China Postdoctoral Science Foundation(No.2019M651342)+2 种基金Shanghai Rising-Star Program(No.18QA1400100)Youth Top-notch Talent Support Program of Shanghai,the Shanghai Committee of Science and Technology,China(No.19520713200)DHU Distinguished Young Professor Program and Fundamental Research Funds for the Central Universities。
文摘Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction between high crystallinity and high surface area,the synthesis of mesoporous SMOs heterojunctions with highly o rdered mesostructures,highly crystallized frameworks,and high surface area remains a huge challenge.In this work,we develop a novel"acid-base pair"adjusted solvent evaporation induced self-assembly(EISA)strategy to prepare highly crystallized ordered mesoporous TiO2/WO3(OM-TiO2/WO3)heterojunctions.The WCl6 and titanium isopropoxide(TIPO)are used as the precursors,respectively,which function as the"acid-base pair",enabling the coassembly with the structure directing agent(PEO-b-PS)into highly ordered meso structures.In addition,PEO-b-PS can be converted to rigid carbon which can protect the meso structures from collapse during the crystallization process.The resultant OM-TiO2/WO3 heterojunctions possess primitive cubic mesostructures,large pore size(~21.1 nm),highly crystalline frameworks and surface area(~98 m2/g).As a sensor for acetone,the obtained OM-TiO2/WO3 show excellent re sponse/recovery perfo rmance(3 s/5 s),good linear dependence,repeatability,selectivity,and long-term stability(35 days).
文摘8wt%WO3/SiO2 metathesis （disproportionation） catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-desorption, scanning electron microscopy （SEM）, X-ray diffraction （XRD）, UV-visible diffuse reflectance spectroscopy （DRS） and scanning transmission electron microscopy-high-angle annular dark field （STEM HAADF）. The results of STEM HAADF showed that WO3 species were not uniformly distributed on the SiO2 support. The experimental results of 8wt%WO3/SiO2 performance in ethene/decene metathesis revealed that the catalytic effect of 8wt%WO3/SiO2 catalyst and coke formation over it were closely related to the support pore structure： The 8wt%WO3/SiO2 catalyst with a more complicated pore structure showed better catalytic performance but the coke deposition rate was also faster.
基金financially supported by the National Key Research and Development Program of China (No. 2016YFC0204300)the National High Technology Research and Development Program of China (No. 2015AA034603)+2 种基金the National Natural Science Foundation of China (Nos. 21333003 and 21571061)the "Shu Guang" Project of the Shanghai Municipal Education Commission (No. 12SG29)the Commission of Science and Technology of Shanghai Municipality (No. 15DZ1205305)
文摘The selective catalytic reduction of NOV with NH3 (NH3-SCR) is a very effective technology to control the emission of NOA, and the thermal stability of NH3-SCR catalyst is very important for removal of NOV from diesel engines. In this work, V2O5/WO3-TiO2 (VWT) and SiO2- doped V2O5/WO3-TiO2 (VWTSi10)) catalysts were prepared by impregnation method and characterized by Brunauer- Emmett-Teller (BET), X-ray diffraction (XRD), Raman, temperature programmed reduction by hydrogen (H2-TPR), X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption by ammonia (NH3- TPD). The doping of SiO2 promotes the thermal stability of V2O5/WO3-TiO? for NH3-SCR significantly. After calcination at 650 °C for 50 h, the operation window of 10% SiO2-doped V2O5/WO3-TiO2 is 220-480 °C, while the maximum NOV conversion on V2O5/WO3-TiO2 is about 77%. The presenee of SiO2 obviously blocks the transformation of TiO2 from anatase to rutile and stabilizes the dispersion of VOv and WO3 on the surface. It is available for the existence of V44 and the amount of surface acid sites increases, which inhabits the NH3 oxidation at the high temperature range and promotes NH3-SCR activity.
文摘The effects of the initial framework SiO2/Al2O3 ratio and temperature on the structural changes of NaY zeolites during hydrothermal treatments are studied. Two samples with different framework SiO2/Al2O3 ratios are subjected to hydrothermal treatment at four different temperatures. For zeolite with a lower initial SiO2/Al2O3 ratio of 4.2, mesopores are easily formed because more framework aluminum is detached. Moreover, two kinds of mesopores are produced at a higher temperature due to the interconnection of vacancies and smaller mesopores. For zeolite with a higher initial SiO2/Al2O3 ratio of 6.0, there are less mesopores formed as compared with the lower initial SiO2/Al2O3 ratio sample, but there are some macropores formed. This may be attributed to the isolation of vacancies and the different distributions of aluminum in the crystal lattice of the zeolite. The experiment data show that NaY with the SiO2/Al2O3 ratio of 6.0 retains a high relative crystallinity during the hydrothermal treatment. This proves that a high framework SiO2/Al2O3 ratio benefits the stability of zeolite.
