CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction（SCR） of NOx with NH3 were p...CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction（SCR） of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping（molar ratio of Ce/Ti = 1/10） in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.展开更多
The phase diagram of HfO_2–TiO_2 system shows that when Ti content is less than 33.0 mol%, HfO_2–TiO_2 system is monoclinic; when Ti content increases from 33.0 mol% to 52.0 mol%, it is orthorhombic; when Ti content...The phase diagram of HfO_2–TiO_2 system shows that when Ti content is less than 33.0 mol%, HfO_2–TiO_2 system is monoclinic; when Ti content increases from 33.0 mol% to 52.0 mol%, it is orthorhombic; when Ti content reaches more than 52.0 mol%, it presents rutile phase. So, we choose the three phases of HfO_2–TiO_2 alloys with different Ti content values. The electronic structures and optical properties of monoclinic, orthorhombic and rutile phases of HfO_2–TiO_2 alloys are obtained by the first-principles generalized gradient approximation（GGA） ＋U approach, and the effects of Ti content and crystal structure on the electronic structures and optical properties of HfO_2–TiO_2 alloys are investigated. By introducing the Coulomb interactions of 5 d orbitals on Hf atom（U_1~d）, those of 3 d orbitals on Ti atom（U_2~d）, and those of 2 p orbitals on O atom（Up） simultaneously, we can improve the calculation values of the band gaps, where U_1~d, U_2~d, and Up values are 8.0 eV, 7.0 eV, and 6.0 eV for both the monoclinic phase and orthorhombic phase, and 8.0 eV, 7.0 eV, and 3.5 eV for the rutile phase. The electronic structures and optical properties of the HfO_2–TiO_2 alloys calculated by GGA ＋U_1~d（U_1~d= 8.0 eV） ＋U_2~d（U_2~d= 7.0 eV） ＋U^p（U^p= 6.0 eV or 3.5 eV） are compared with available experimental results.展开更多
The adsorption of mesoporous Fe3O4–SiO2–TiO2(MFST), which can be separated easily from solution by a magnet, for the removal of methyl orange(MO) was investigated. The nitrogen adsorption–desorption measurement sho...The adsorption of mesoporous Fe3O4–SiO2–TiO2(MFST), which can be separated easily from solution by a magnet, for the removal of methyl orange(MO) was investigated. The nitrogen adsorption–desorption measurement shows successful synthesis of MFST with an average pore size of 3.8 nm and a large specific surface area of55 m2·g-1. About 95% adsorption percentage of MO is achieved with an initial concentration of 10 mg·L-1in the dark and the MFST exhibits superior adsorption ability under acid conditions. The adsorption data fit well with the pseudo-second order model for adsorption. After 4 cycles, the adsorption rate for MO remains 74% in the dark and the MFST can be recovered in a magnetic field with a recovery of about 80 %(by mass). It demonstrates that the samples have significant value on applications of wastewater treatment.展开更多
A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless depo...A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless deposition method and evaluated for the deep oxidation of n-hexane as a model VOCs. The results show that the CeO_(2)and TiOxnanoparticles can highly disperse into each other and form Ce_(2)Ti_(2)O_(7)solid solution with appropriate Ce/Ti molar ratio, which significantly improves their redox ability by enhancing the interaction between CeO_(2)and TiO_(x). The dispersibility of Pt species can also be adjusted by altering the Ce/Ti molar ratio, and Pt/CeTi-2/1 catalyst with Ce/Ti molar ratio of 2:1 exhibits the best Pt dispersibility that Pt species mainly exist as Pt single atoms. The high dispersion of Pt species in the Pt/CeO_(2)-TiO_(2)catalysts would promote the catalytic activity of VOCs oxidation with low T90% values(1000 ppm, GHSV = 15,000 h^(-1)), such as for n-hexane degradation with T90% of 139℃. The characterizations reveal that the superior activity is mainly related to possessing the more Pt2+species,adsorbed oxygen species and higher low-temperature reducibility owing to the strong interaction between highly dispersed Pt species and CeO_(2)-TiO_(2)as well as the promoted migration of lattice oxygen by the formation of more Ce_(2)Ti_(2)O_(7)species. Furthermore, the Pt/CeTi-2/1 catalyst also exhibits excellent stability for chlorinated and other non-chlorinated VOCs oxidation, making it very promising for real application under various operating conditions.展开更多
In this paper, in-situ coagulation of 0.9Al_2O_3–0.1TiO_2 suspension and microwave dielectric properties of 0.9Al_2O_3–0.1TiO_2 ceramics prepared by a novel direct coagulation casting via high valence counter ions(D...In this paper, in-situ coagulation of 0.9Al_2O_3–0.1TiO_2 suspension and microwave dielectric properties of 0.9Al_2O_3–0.1TiO_2 ceramics prepared by a novel direct coagulation casting via high valence counter ions(DCC-HVCI) method were proposed. The 0.9Al_2O_3–0.1TiO_2 suspension could be coagulated via controlled release of calcium ions from calcium iodate at an elevated temperature. The influence of tri-ammonium citrate(TAC) content, solid loading, and calcium iodate content on the rheological properties of the suspension was investigated. In addition, the influence of coagulation temperature on coagulation time and properties of green bodies was also studied. It was found that the stable 0.9Al_2O_3–0.1TiO_2 suspension could be successfully prepared by adding 0.3 wt% TAC and adjusting pH value to 10–12 at room temperature. 0.9Al_2O_3–0.1TiO_2 green bodies with uniform microstructures were coagulated by adding 8.0 g/L calcium iodate after treating at 70 ℃ for 1 h. 0.9Al_2O_3–0.1TiO_2 ceramics, sintered at 1500 ℃ for 4 h and annealed at 1100 ℃ for 5 h, showed uniform microstructures with density of 3.62±0.02 g/cm^3. The microwave dielectric properties of 0.9Al_2O_3–0.1TiO_2 ceramics prepared by DCC-HVCI method were: ε_r = 11.26±0.06, Q×f = 11569± 629 GHz, τ_t = 0.93±0.60 ppm/℃. The DCC-HVCI method is a novel and promising route without binder removal process to prepare complex-shaped microwave dielectric ceramics with uniform microstructures and good microwave dielectric properties.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos. 21376261, 21173270, 21177160)the National Hi-Tech Research and Development Program (863) of China (No. 2013AA065302)+2 种基金the Beijing Natural Science Foundation (2142027)the Doctoral Selection Fund (No. 20130007110007)the China University of Petroleum Fund (No. KYJJ2012-06-31)
文摘CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction（SCR） of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping（molar ratio of Ce/Ti = 1/10） in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11672087,11502058,and 11402252)
文摘The phase diagram of HfO_2–TiO_2 system shows that when Ti content is less than 33.0 mol%, HfO_2–TiO_2 system is monoclinic; when Ti content increases from 33.0 mol% to 52.0 mol%, it is orthorhombic; when Ti content reaches more than 52.0 mol%, it presents rutile phase. So, we choose the three phases of HfO_2–TiO_2 alloys with different Ti content values. The electronic structures and optical properties of monoclinic, orthorhombic and rutile phases of HfO_2–TiO_2 alloys are obtained by the first-principles generalized gradient approximation（GGA） ＋U approach, and the effects of Ti content and crystal structure on the electronic structures and optical properties of HfO_2–TiO_2 alloys are investigated. By introducing the Coulomb interactions of 5 d orbitals on Hf atom（U_1~d）, those of 3 d orbitals on Ti atom（U_2~d）, and those of 2 p orbitals on O atom（Up） simultaneously, we can improve the calculation values of the band gaps, where U_1~d, U_2~d, and Up values are 8.0 eV, 7.0 eV, and 6.0 eV for both the monoclinic phase and orthorhombic phase, and 8.0 eV, 7.0 eV, and 3.5 eV for the rutile phase. The electronic structures and optical properties of the HfO_2–TiO_2 alloys calculated by GGA ＋U_1~d（U_1~d= 8.0 eV） ＋U_2~d（U_2~d= 7.0 eV） ＋U^p（U^p= 6.0 eV or 3.5 eV） are compared with available experimental results.
基金Supported by the National Natural Science Foundation of China(2011011013-2)the Youth Foundation of Science and Technology Agency of Shanxi Province,China(2011021020-2)
文摘The adsorption of mesoporous Fe3O4–SiO2–TiO2(MFST), which can be separated easily from solution by a magnet, for the removal of methyl orange(MO) was investigated. The nitrogen adsorption–desorption measurement shows successful synthesis of MFST with an average pore size of 3.8 nm and a large specific surface area of55 m2·g-1. About 95% adsorption percentage of MO is achieved with an initial concentration of 10 mg·L-1in the dark and the MFST exhibits superior adsorption ability under acid conditions. The adsorption data fit well with the pseudo-second order model for adsorption. After 4 cycles, the adsorption rate for MO remains 74% in the dark and the MFST can be recovered in a magnetic field with a recovery of about 80 %(by mass). It demonstrates that the samples have significant value on applications of wastewater treatment.
基金supported by a grant from the National Key Research and Development Program of China (2016YFC0204300)the National Nature Science Foundation of China (21477109)。
文摘A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless deposition method and evaluated for the deep oxidation of n-hexane as a model VOCs. The results show that the CeO_(2)and TiOxnanoparticles can highly disperse into each other and form Ce_(2)Ti_(2)O_(7)solid solution with appropriate Ce/Ti molar ratio, which significantly improves their redox ability by enhancing the interaction between CeO_(2)and TiO_(x). The dispersibility of Pt species can also be adjusted by altering the Ce/Ti molar ratio, and Pt/CeTi-2/1 catalyst with Ce/Ti molar ratio of 2:1 exhibits the best Pt dispersibility that Pt species mainly exist as Pt single atoms. The high dispersion of Pt species in the Pt/CeO_(2)-TiO_(2)catalysts would promote the catalytic activity of VOCs oxidation with low T90% values(1000 ppm, GHSV = 15,000 h^(-1)), such as for n-hexane degradation with T90% of 139℃. The characterizations reveal that the superior activity is mainly related to possessing the more Pt2+species,adsorbed oxygen species and higher low-temperature reducibility owing to the strong interaction between highly dispersed Pt species and CeO_(2)-TiO_(2)as well as the promoted migration of lattice oxygen by the formation of more Ce_(2)Ti_(2)O_(7)species. Furthermore, the Pt/CeTi-2/1 catalyst also exhibits excellent stability for chlorinated and other non-chlorinated VOCs oxidation, making it very promising for real application under various operating conditions.
基金supported by National Natural Science Foundation of China(No.51501066)China Postdoctoral Science Foundation(Nos.2015M572136,2017T100550,and 2016M602290)the Fundamental Research Funds for the Central University(No.2017JYCXJJ002)
文摘In this paper, in-situ coagulation of 0.9Al_2O_3–0.1TiO_2 suspension and microwave dielectric properties of 0.9Al_2O_3–0.1TiO_2 ceramics prepared by a novel direct coagulation casting via high valence counter ions(DCC-HVCI) method were proposed. The 0.9Al_2O_3–0.1TiO_2 suspension could be coagulated via controlled release of calcium ions from calcium iodate at an elevated temperature. The influence of tri-ammonium citrate(TAC) content, solid loading, and calcium iodate content on the rheological properties of the suspension was investigated. In addition, the influence of coagulation temperature on coagulation time and properties of green bodies was also studied. It was found that the stable 0.9Al_2O_3–0.1TiO_2 suspension could be successfully prepared by adding 0.3 wt% TAC and adjusting pH value to 10–12 at room temperature. 0.9Al_2O_3–0.1TiO_2 green bodies with uniform microstructures were coagulated by adding 8.0 g/L calcium iodate after treating at 70 ℃ for 1 h. 0.9Al_2O_3–0.1TiO_2 ceramics, sintered at 1500 ℃ for 4 h and annealed at 1100 ℃ for 5 h, showed uniform microstructures with density of 3.62±0.02 g/cm^3. The microwave dielectric properties of 0.9Al_2O_3–0.1TiO_2 ceramics prepared by DCC-HVCI method were: ε_r = 11.26±0.06, Q×f = 11569± 629 GHz, τ_t = 0.93±0.60 ppm/℃. The DCC-HVCI method is a novel and promising route without binder removal process to prepare complex-shaped microwave dielectric ceramics with uniform microstructures and good microwave dielectric properties.
