Aminopropyltriethoxysilane (AM), 3-ethyldiaminopropyltrimethoxysilane (ED) and 3-piperazinylpropyltriethoxysilane (PZ), were used to chemically couple with the silanol groups of calcined hexagonal and hexagonal-like m...Aminopropyltriethoxysilane (AM), 3-ethyldiaminopropyltrimethoxysilane (ED) and 3-piperazinylpropyltriethoxysilane (PZ), were used to chemically couple with the silanol groups of calcined hexagonal and hexagonal-like mesoporous silica SBA-3 and HMS, respectively, to produce functionalised alkaline mesoporous materials. The increase in the dosage of organosilanes, or in reaction temperature, or in the humidity (i.e., water content) of support, is favorable to the grafting of functional molecules on the surface. When functionalization conditions are the same, the order of loadings on SBA-3 and DDA-HMS is ED>AM>PZ. However, on ODA-HMS, the loading of AM is similar to that of ED.展开更多
Tungsten-containing hexagonal mesoporous silica (W-HMS) supported tungsten oxide catalysts (WOx/W-HMS) was prepared for the selective oxidation of cyclopentene with aqueous hydrogen peroxide to glutaraldehyde. X-r...Tungsten-containing hexagonal mesoporous silica (W-HMS) supported tungsten oxide catalysts (WOx/W-HMS) was prepared for the selective oxidation of cyclopentene with aqueous hydrogen peroxide to glutaraldehyde. X-ray diffraction (XRD) results indicated that the crystal form of the active phase (tungsten oxide) of the WOx/W-HMS catalysts was dependent on the W loading and calcination temperature. X-ray photoelectron spec- troscopy (XPS) analysis revealed that the dispersed tungsten oxides on the surface of W-HMS support consisted of a mixture of W(V) and W(VI). It was found that a high content of amorphous W species in (5+) oxidation state resuited in the high catalytic activity. When the W loading was up to 12% (by mass) or the catalyst precursor was treated at temperature of 623 K, the catalytic activity decreased due to the presence of WO3 crystallites and the oxidation of W(V) to W(VI) on the catalyst surface. Furthermore, NH3-temperature-programmed-desorption (NH3-TPD) analysis showed that the effects of W loading and calcination temperature on the acidity of the catalysts were related to the catalytic activity. A high selectivity of 80.2% for glutaraldehyde with a complete conversion of cyclopentene was obtained over 8%WOx/W-HMS catalyst calcined at 573 K after 14 h of reaction.展开更多
Reverse water gas shift(RWGS)reaction is a crucial process in CO_(2)utilization.Herein,Ni-and NiCe-containing hexagonal mesoporous silica(Ni-HMS and NiCe-HMS)catalysts were synthesized using an insitu one-pot method a...Reverse water gas shift(RWGS)reaction is a crucial process in CO_(2)utilization.Herein,Ni-and NiCe-containing hexagonal mesoporous silica(Ni-HMS and NiCe-HMS)catalysts were synthesized using an insitu one-pot method and applied for RWGS reaction.At certain reaction temperatures 500-750℃,Ni-HMS samples displayed a higher selectivity to the preferable CO than that of conventionally impregnated Ni/HMS catalyst.This could be originated from the smaller NiO nanoparticles over Ni-HMS catalyst.NiCe-HMS exhibited higher activity compared to Ni-HMS.The catalysts were characterized by means of TEM,XPS,XRD,H_(2)-TPR,CO_(2)-TPD,EPR and N_(2) adsorption-desortion technology.It was found that introduction of Ce created high concentration of oxygen vacancies,served as the active site for activating CO_(2).Also,this work analyzed the effect of the H_(2)/CO_(2)molar ratio on the best NiCe-HMS.When reaction gas H_(2)/CO_(2)molar ratio was 4 significantly decreased the selectivity to CO at low temperature,but triggered a higher CO_(2)conversion which is close to the equilibrium.展开更多
文摘Aminopropyltriethoxysilane (AM), 3-ethyldiaminopropyltrimethoxysilane (ED) and 3-piperazinylpropyltriethoxysilane (PZ), were used to chemically couple with the silanol groups of calcined hexagonal and hexagonal-like mesoporous silica SBA-3 and HMS, respectively, to produce functionalised alkaline mesoporous materials. The increase in the dosage of organosilanes, or in reaction temperature, or in the humidity (i.e., water content) of support, is favorable to the grafting of functional molecules on the surface. When functionalization conditions are the same, the order of loadings on SBA-3 and DDA-HMS is ED>AM>PZ. However, on ODA-HMS, the loading of AM is similar to that of ED.
文摘Tungsten-containing hexagonal mesoporous silica (W-HMS) supported tungsten oxide catalysts (WOx/W-HMS) was prepared for the selective oxidation of cyclopentene with aqueous hydrogen peroxide to glutaraldehyde. X-ray diffraction (XRD) results indicated that the crystal form of the active phase (tungsten oxide) of the WOx/W-HMS catalysts was dependent on the W loading and calcination temperature. X-ray photoelectron spec- troscopy (XPS) analysis revealed that the dispersed tungsten oxides on the surface of W-HMS support consisted of a mixture of W(V) and W(VI). It was found that a high content of amorphous W species in (5+) oxidation state resuited in the high catalytic activity. When the W loading was up to 12% (by mass) or the catalyst precursor was treated at temperature of 623 K, the catalytic activity decreased due to the presence of WO3 crystallites and the oxidation of W(V) to W(VI) on the catalyst surface. Furthermore, NH3-temperature-programmed-desorption (NH3-TPD) analysis showed that the effects of W loading and calcination temperature on the acidity of the catalysts were related to the catalytic activity. A high selectivity of 80.2% for glutaraldehyde with a complete conversion of cyclopentene was obtained over 8%WOx/W-HMS catalyst calcined at 573 K after 14 h of reaction.
基金the Chengdu University of Technology Teachers Development Research Fund (No. 10912-2019KYQD07266)National Natural Science Foundation of China (No. 21806015) for financial support
文摘Reverse water gas shift(RWGS)reaction is a crucial process in CO_(2)utilization.Herein,Ni-and NiCe-containing hexagonal mesoporous silica(Ni-HMS and NiCe-HMS)catalysts were synthesized using an insitu one-pot method and applied for RWGS reaction.At certain reaction temperatures 500-750℃,Ni-HMS samples displayed a higher selectivity to the preferable CO than that of conventionally impregnated Ni/HMS catalyst.This could be originated from the smaller NiO nanoparticles over Ni-HMS catalyst.NiCe-HMS exhibited higher activity compared to Ni-HMS.The catalysts were characterized by means of TEM,XPS,XRD,H_(2)-TPR,CO_(2)-TPD,EPR and N_(2) adsorption-desortion technology.It was found that introduction of Ce created high concentration of oxygen vacancies,served as the active site for activating CO_(2).Also,this work analyzed the effect of the H_(2)/CO_(2)molar ratio on the best NiCe-HMS.When reaction gas H_(2)/CO_(2)molar ratio was 4 significantly decreased the selectivity to CO at low temperature,but triggered a higher CO_(2)conversion which is close to the equilibrium.