A series of sulfided PtMo/ γ Al 2O 3 catalysts[ w (Mo)=9.0%] with different contents of Pt were characterized by using low temperature FTIR spectroscopy of adsorbed CO, while their HDS activity was investigated with ...A series of sulfided PtMo/ γ Al 2O 3 catalysts[ w (Mo)=9.0%] with different contents of Pt were characterized by using low temperature FTIR spectroscopy of adsorbed CO, while their HDS activity was investigated with thiophene as a model substrate. Experimentally, it was found that no existence of the bands related to the surface complexes of Al 3+ ←CO and Pt 0←CO→Pt 0 was observed at 77 K and that the rate of the thiophene HDS reaction(573 K) is well linearly proportional to the area of the Pt 0←CO band at 2 093 cm -1 with a higher extrapolated HDS rate compared to that of sulfided Mo/ γ Al 2O 3 catalyst at the zero content of platinum. On the basis of the results here, the conclusion may be made that the active monolayer phase of Pt Mo S may be formed over sulfided PtMo/ γ Al 2O 3 catalysts during the sulfidation process and that both Mo 2+ and Pt 0 sites for CO adsorption should be the active reaction centers of thiophene HDS.展开更多
Three-dimensionally ordered macro-/mesoporous alumina(3DOM Al2O3)-supported cobalt oxide and platinum nanocatalysts(xPt/yCo3O4/3DOM Al2O3,Pt mass fraction(x%)= 0-1.4%,Co3O4 mass fraction(y%) = 0-9.2%) were pre...Three-dimensionally ordered macro-/mesoporous alumina(3DOM Al2O3)-supported cobalt oxide and platinum nanocatalysts(xPt/yCo3O4/3DOM Al2O3,Pt mass fraction(x%)= 0-1.4%,Co3O4 mass fraction(y%) = 0-9.2%) were prepared using poly(methyl methacrylate) templating,incipient wetness impregnation and polyvinyl alcohol-protected reduction.The resulting xPt/yCo3O4/3DOM Al2O3 samples displayed a high-quality 3DOM architecture with macropores(180-200 nm in diameter) and mesopores(4-6 nm in diameter) together with surface areas in the range of 94 to 102m^2/g.Using these techniques,Co3O4 nanoparticles(NPs,18.3 nm) were loaded on the 3DOM Al2O3 surface,after which Pt NPs(2.3-2.5 nm) were uniformly dispersed on theyCo3O4/3DOM Al2O3.The1.3Pt/8.9Co3O4/3DOM Al2O3 exhibited the best performance for toluene oxidation,with a T(90%) value(the temperature required to achieve 90%toluene conversion) of 160 ℃ at a space velocity of20000 mL g^(-1) h^(-1).It is concluded that the excellent catalytic performance of the 1.3Pt/8.9Co3O4/3DOM Al2O3 is owing to well-dispersed Pt NPs,the high concentration of adsorbed oxygen species,good low-temperature reducibility,and strong interaction between the Pt and Co3O4 NPs,as well as the unique bimodal porous structure of the support.展开更多
Featuring an assembly of identical pores, through-pore anodic alumina (AAO) makes an ideal monolith-like cat- alyst support for volatile organic compound (VOC) combustion. This work employs the oxidation of toluen...Featuring an assembly of identical pores, through-pore anodic alumina (AAO) makes an ideal monolith-like cat- alyst support for volatile organic compound (VOC) combustion. This work employs the oxidation of toluene as a model reaction to investigate the applicability of AAO supported Pt catalysts in VOC catalytic combustion. In order to modify the microstructure of AAO, some AAO samples were exposed to hot water treatment (HWT) firstly. Re- sults show that the optimum HWT time is 18 h. Pt/HWT18 gives a toluene conversion of95%; at 200 ℃, which is comparable to the initial activity of commercial γ-A1203 particle supported Pt catalyst. Considering its confine- ment effect for the supported metal and its monolith-like compact unit, AAO support offers potential applications in VOC catalytic combustion.展开更多
文摘A series of sulfided PtMo/ γ Al 2O 3 catalysts[ w (Mo)=9.0%] with different contents of Pt were characterized by using low temperature FTIR spectroscopy of adsorbed CO, while their HDS activity was investigated with thiophene as a model substrate. Experimentally, it was found that no existence of the bands related to the surface complexes of Al 3+ ←CO and Pt 0←CO→Pt 0 was observed at 77 K and that the rate of the thiophene HDS reaction(573 K) is well linearly proportional to the area of the Pt 0←CO band at 2 093 cm -1 with a higher extrapolated HDS rate compared to that of sulfided Mo/ γ Al 2O 3 catalyst at the zero content of platinum. On the basis of the results here, the conclusion may be made that the active monolayer phase of Pt Mo S may be formed over sulfided PtMo/ γ Al 2O 3 catalysts during the sulfidation process and that both Mo 2+ and Pt 0 sites for CO adsorption should be the active reaction centers of thiophene HDS.
基金supported by the National High Technology Research and Development Program of China(863 Program,2015AA034603)the National Natural Science Foundation of China(21377008)Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions
文摘Three-dimensionally ordered macro-/mesoporous alumina(3DOM Al2O3)-supported cobalt oxide and platinum nanocatalysts(xPt/yCo3O4/3DOM Al2O3,Pt mass fraction(x%)= 0-1.4%,Co3O4 mass fraction(y%) = 0-9.2%) were prepared using poly(methyl methacrylate) templating,incipient wetness impregnation and polyvinyl alcohol-protected reduction.The resulting xPt/yCo3O4/3DOM Al2O3 samples displayed a high-quality 3DOM architecture with macropores(180-200 nm in diameter) and mesopores(4-6 nm in diameter) together with surface areas in the range of 94 to 102m^2/g.Using these techniques,Co3O4 nanoparticles(NPs,18.3 nm) were loaded on the 3DOM Al2O3 surface,after which Pt NPs(2.3-2.5 nm) were uniformly dispersed on theyCo3O4/3DOM Al2O3.The1.3Pt/8.9Co3O4/3DOM Al2O3 exhibited the best performance for toluene oxidation,with a T(90%) value(the temperature required to achieve 90%toluene conversion) of 160 ℃ at a space velocity of20000 mL g^(-1) h^(-1).It is concluded that the excellent catalytic performance of the 1.3Pt/8.9Co3O4/3DOM Al2O3 is owing to well-dispersed Pt NPs,the high concentration of adsorbed oxygen species,good low-temperature reducibility,and strong interaction between the Pt and Co3O4 NPs,as well as the unique bimodal porous structure of the support.
基金Supported by the National Natural Science Foundation of China(21106189,21036009)the Natural Science Foundation(S2011040001767)the Foundation from the Educational Commission(LYM11004)of Guangdong Province
文摘Featuring an assembly of identical pores, through-pore anodic alumina (AAO) makes an ideal monolith-like cat- alyst support for volatile organic compound (VOC) combustion. This work employs the oxidation of toluene as a model reaction to investigate the applicability of AAO supported Pt catalysts in VOC catalytic combustion. In order to modify the microstructure of AAO, some AAO samples were exposed to hot water treatment (HWT) firstly. Re- sults show that the optimum HWT time is 18 h. Pt/HWT18 gives a toluene conversion of95%; at 200 ℃, which is comparable to the initial activity of commercial γ-A1203 particle supported Pt catalyst. Considering its confine- ment effect for the supported metal and its monolith-like compact unit, AAO support offers potential applications in VOC catalytic combustion.