V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for N...V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.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
A lithium ion conductive solid electrolyte, L20-AI203-TiO2-SiO2-P20s glass with NASICON- type structure have been synthesized and transformed into glass-ceramic through thermal-treatment at various temperatures from 7...A lithium ion conductive solid electrolyte, L20-AI203-TiO2-SiO2-P20s glass with NASICON- type structure have been synthesized and transformed into glass-ceramic through thermal-treatment at various temperatures from 700 to 1 000 ~C for 12 h. The differential scanning calorimetry (DSC), X-ray diffraction (XRD), scanning electron microscopy (SEM) and complex impedance techniques were employed to characterize the samples. The experimental results indicated that the capability of glass forming in this system is superior to that of L20-A1203-TiO2-PzO~. The glass has an amorphous structure and resultant glass-ceramic mainly consisting of LiTi2(PO4)3 phases. Impurity phases AIPO4, TiO2, TiP207 and unidentified phase were observed. With the enhanced heat-treatment temperature, grain grew gradually and lithium ion conductivity of glass-ceramics increased accordingly, the related impedance semicircles were depressed gradually and even disappeared, which could be analytically explained by the coordinate action of the 'Constant phase element' (CPE) model and the 'Concept of Mismatch and Relaxation' model (CMR). When the sample is devitrified at 1 000 ~C, the maximum room temperature lithium ion conductivity comes up to 4.1 x 10-4 S/cm, which is suitable for the application as an electrolyte of all-solid-state lithium batteries.展开更多
Li4Ti5012 (LTO) with rich R-TiO2 (17.06, 23.69, and 34.42 wt%), namely, R-TiO2@Li4Ti5O12 composites, were synthesized using the hydrothermal method and tetrabutyl titanate (TBT) as the precursor. Rietveld refinement o...Li4Ti5012 (LTO) with rich R-TiO2 (17.06, 23.69, and 34.42 wt%), namely, R-TiO2@Li4Ti5O12 composites, were synthesized using the hydrothermal method and tetrabutyl titanate (TBT) as the precursor. Rietveld refinement of X-ray diffraction (XRD) results show that the proportion of Li occupying 16d sites is extraordinary low and the lattice constants of LTO and R-TiO2 change with the ritanium dioxide content. EIS measurements showed that with in creasing R-TiO2 content, both its charge transfer impedance (Rct) and lithium ion diffusion coefficient (DLi) decreased. The changes of Rct and DLi caused by the increase of titanium dioxide content have synergic-antagonistic effects on the rate and cycle properties of Li4Ti5012. The rate performance is positively related to DLi, while the cycle property is negatively correlated with Rct, indicati ng that the rate performs nee is mainly related to DLi, while Rct more significantly affects the cycle performance. LTO-RT-17.06% exhibited excellent rate properties, especially under a high current density (5.0 C, 132.5 mAh/g) and LTO-RT-34.42% showed superior long-term cycle performance (0.012% capacity loss per cycle) compared to that of LTO-RT-17.06% and LTO-RT-23.69%.展开更多
The lithium ion-conductive solid electrolyte in the oxide systems of Li2O-TiO2-SiO2-P2O5 and Li2O-TiO2-Al2O3-P2O5 was prepared by solid-state reaction. The electrolyte pellets by cold-pressing method is 13 mm in diame...The lithium ion-conductive solid electrolyte in the oxide systems of Li2O-TiO2-SiO2-P2O5 and Li2O-TiO2-Al2O3-P2O5 was prepared by solid-state reaction. The electrolyte pellets by cold-pressing method is 13 mm in diameter, about 1 mm in thickness. Phase identification and surface morphology of the products were carried out by X-ray diffraction and scanning electron microscopy. Ionic conductivity of the pellets was investigated through AC impedance. The results show that adulterate other cations can improve the ionic conductivity of the solid electrolyte. The maximum ionic conductivity in the samples is 9.912 × 10-4 S·cm-1 in the Li2O-TiO2-SiO2-P2O5 system.展开更多
采用溶胶-凝胶的方法低温制备石榴石结构的固体电解质Li5La3Ta2O12,并用其包覆Li Mn2O4来改善材料的电化学性能。通过XRD,SEM和TEM等表征手段对材料的结构和形貌进行分析,并通过恒电流充放电、循环伏安、交流阻抗等测试分析材料的电化...采用溶胶-凝胶的方法低温制备石榴石结构的固体电解质Li5La3Ta2O12,并用其包覆Li Mn2O4来改善材料的电化学性能。通过XRD,SEM和TEM等表征手段对材料的结构和形貌进行分析,并通过恒电流充放电、循环伏安、交流阻抗等测试分析材料的电化学性能。研究结果表明:Li5La3Ta2O12包覆的Li Mn2O4材料与未包覆的材料相比,其电化学性能得到明显改善,经过150次循环后包覆材料的放电比容量保持率为92%,在高倍率10C(C为倍率)下包覆材料放电比容量为61.2 m A·h/g,而未包覆材料放电比容量仅为40.7 m A·h/g;包覆Li5La3Ta2O12后,Li Mn2O4的阻抗明显减小,大幅度提高了其循环性能和倍率性能。展开更多
基金supported by the National Natural Science Foundation of China (51372137)the National High Technology Research and Development Program of China (863 Program,2015AA034603)~~
摘要V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.
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)
摘要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.
基金National Basic Research Program of China (No.2009CB939704)National Natural Science Foundation of China (Nos.51032005, 60808024)the Fundamental Research Funds for the Central Universities (Wuhan University of Technology)
摘要A lithium ion conductive solid electrolyte, L20-AI203-TiO2-SiO2-P20s glass with NASICON- type structure have been synthesized and transformed into glass-ceramic through thermal-treatment at various temperatures from 700 to 1 000 ~C for 12 h. The differential scanning calorimetry (DSC), X-ray diffraction (XRD), scanning electron microscopy (SEM) and complex impedance techniques were employed to characterize the samples. The experimental results indicated that the capability of glass forming in this system is superior to that of L20-A1203-TiO2-PzO~. The glass has an amorphous structure and resultant glass-ceramic mainly consisting of LiTi2(PO4)3 phases. Impurity phases AIPO4, TiO2, TiP207 and unidentified phase were observed. With the enhanced heat-treatment temperature, grain grew gradually and lithium ion conductivity of glass-ceramics increased accordingly, the related impedance semicircles were depressed gradually and even disappeared, which could be analytically explained by the coordinate action of the 'Constant phase element' (CPE) model and the 'Concept of Mismatch and Relaxation' model (CMR). When the sample is devitrified at 1 000 ~C, the maximum room temperature lithium ion conductivity comes up to 4.1 x 10-4 S/cm, which is suitable for the application as an electrolyte of all-solid-state lithium batteries.
基金financially supported by the National Natural Science Foundation of China(No.51641206)Shandong Natural Science Foundation Project(No.ZR2015EM013)+1 种基金Special Funds for Independent Innovation and Transformation of Achievements in Shandong Province(No.2014CGZH0911)National Key R&D Program of China(No.2016YFB0100508)
摘要Li4Ti5012 (LTO) with rich R-TiO2 (17.06, 23.69, and 34.42 wt%), namely, R-TiO2@Li4Ti5O12 composites, were synthesized using the hydrothermal method and tetrabutyl titanate (TBT) as the precursor. Rietveld refinement of X-ray diffraction (XRD) results show that the proportion of Li occupying 16d sites is extraordinary low and the lattice constants of LTO and R-TiO2 change with the ritanium dioxide content. EIS measurements showed that with in creasing R-TiO2 content, both its charge transfer impedance (Rct) and lithium ion diffusion coefficient (DLi) decreased. The changes of Rct and DLi caused by the increase of titanium dioxide content have synergic-antagonistic effects on the rate and cycle properties of Li4Ti5012. The rate performance is positively related to DLi, while the cycle property is negatively correlated with Rct, indicati ng that the rate performs nee is mainly related to DLi, while Rct more significantly affects the cycle performance. LTO-RT-17.06% exhibited excellent rate properties, especially under a high current density (5.0 C, 132.5 mAh/g) and LTO-RT-34.42% showed superior long-term cycle performance (0.012% capacity loss per cycle) compared to that of LTO-RT-17.06% and LTO-RT-23.69%.
摘要The lithium ion-conductive solid electrolyte in the oxide systems of Li2O-TiO2-SiO2-P2O5 and Li2O-TiO2-Al2O3-P2O5 was prepared by solid-state reaction. The electrolyte pellets by cold-pressing method is 13 mm in diameter, about 1 mm in thickness. Phase identification and surface morphology of the products were carried out by X-ray diffraction and scanning electron microscopy. Ionic conductivity of the pellets was investigated through AC impedance. The results show that adulterate other cations can improve the ionic conductivity of the solid electrolyte. The maximum ionic conductivity in the samples is 9.912 × 10-4 S·cm-1 in the Li2O-TiO2-SiO2-P2O5 system.
摘要采用溶胶-凝胶的方法低温制备石榴石结构的固体电解质Li5La3Ta2O12,并用其包覆Li Mn2O4来改善材料的电化学性能。通过XRD,SEM和TEM等表征手段对材料的结构和形貌进行分析,并通过恒电流充放电、循环伏安、交流阻抗等测试分析材料的电化学性能。研究结果表明:Li5La3Ta2O12包覆的Li Mn2O4材料与未包覆的材料相比,其电化学性能得到明显改善,经过150次循环后包覆材料的放电比容量保持率为92%,在高倍率10C(C为倍率)下包覆材料放电比容量为61.2 m A·h/g,而未包覆材料放电比容量仅为40.7 m A·h/g;包覆Li5La3Ta2O12后,Li Mn2O4的阻抗明显减小,大幅度提高了其循环性能和倍率性能。