Structural and compositional design of core-shell structure is an effective strategy towards enhanced catalysis.Herein,amorphous MnO2 nanosheets and K+-intercalated layered MnO2 nanosheets are controllably assembled o...Structural and compositional design of core-shell structure is an effective strategy towards enhanced catalysis.Herein,amorphous MnO2 nanosheets and K+-intercalated layered MnO2 nanosheets are controllably assembled over Fe2O3 spindles,in which the MnO2 nanosheets are perpendicularly anchored to the surface of Fe2O3.Such a core shell structure contributes to a high specific surface area and abundant pore channels on the surface of catalysts.In addition,the existence of K+provides large numbers of basic sites and restrains the formation of unpleasant(Fe1-xMnx)3O4.Benefiting from the merits in structure and composition,CO adsorption is enhanced and remaining time of intermediates is prolonged on the surfaces of catalysts during the Fischer–Tropsch synthesis(FTS),facilitating to the formation of active iron carbides and C–C coupling reactions.Resultantly,the Fe2O3@K+-Mn O2 shows both a high CO conversion of 82.3%and a high C5+ selectivity of 73.1%.The present study provides structural and compositional rationales on design high-performance catalysts towards FTS.展开更多
Single-wall carbon nanotubes （SWNTs） with high surface area were synthesized over nanoporous Co-Mo/MgO by a chemical vapor deposition （CVD） method. The SWNTs were used as catalyst support for selective hydrogenati...Single-wall carbon nanotubes （SWNTs） with high surface area were synthesized over nanoporous Co-Mo/MgO by a chemical vapor deposition （CVD） method. The SWNTs were used as catalyst support for selective hydrogenation of syngas to hydrocarbons. Here an extensive study of Fischer-Tropsch synthesis （FTS） on CNT-supported cobalt catalysts with different amounts of cobalt loading up to 40 wt% is reported. The catalysts were characterized by different methods including N2 adsorption-desorption, X-ray diffraction, hydrogen chemisorption, inductively coupled plasma （ICP） and temperature-programmed reduction. Enhancement of the reducibility of Co3O4 to CoO, CoO to Co° and small cobalt oxide particles, dispersion of the cobalt, and activity and selectivity of FTS were investigated and compared with a conventional support. The CNT supported catalysts achieve a high dispersion and high loading of the active metal, cobalt in particular, so that the bulk formation of cobalt metal, which tends to occur in conventional support, can be avoided. The results showed that the specific activity of CNT supported catalysts increase significantly （there is a two fold increase in CO Conversion per gram of the active metal） with respect to the conventional supported catalyst.展开更多
The effect of reduction procedure on catalyst properties, activity and products selectivity of ruthenium-promoted Co/γ-Al2O3 catalyst in Fischer-Tropsch synthesis （FTS） was investigated. Catalyst samples were redu...The effect of reduction procedure on catalyst properties, activity and products selectivity of ruthenium-promoted Co/γ-Al2O3 catalyst in Fischer-Tropsch synthesis （FTS） was investigated. Catalyst samples were reduced with different reduction gas compositions and passivated before being characterized by TPR and XRD techniques. Different activity and product selectivity analyses were also performed. These results showed that the catalyst dispersion, particle size, and the degree of reduction changed with different reduction gas compositions, which were resulted from the water partial pressures in reduction process that give varying degrees of interaction with the support. It has been suggested that the FTS activity of cobalt catalyst was directly dependent on the catalyst reducibility. A reduction gas with a molar ratio of H2Prle = 1 was used to prevent the formation of Co-support compound during catalyst reduction.展开更多
Ordered SBA-15 mesoporous silica with incorporated titanium was successfully synthesized via a onepot hydrothermal crystallization method.The characterization including powder X-ray diffraction,Brunauer–Emmett–Telle...Ordered SBA-15 mesoporous silica with incorporated titanium was successfully synthesized via a onepot hydrothermal crystallization method.The characterization including powder X-ray diffraction,Brunauer–Emmett–Teller,transmission electron microscope,temperatureprogrammed reduction,temperature-programmed desorption,Fourier transform infrared and ultraviolet-visible-near infrared spectrometer was performed to explore the physical and chemical structures of both the supports and the catalysts.The results showed that titanium was successfully incorporated into the mesoporous silica framework with a limited amount of titanium(Si/Ti>20),and the mesoporous structure was retained.However,the increased titanium content inevitably resulted in the formation of anatase TiO2 particles on the support surface.The increased incorporated titanium strengthened the interactions between cobalt species and supports,which was favorable for the cobalt species dispersion,despite the limited cobalt oxide reducibility.The enhanced metalsupport interactions were beneficial for the CO/H2 ratio at the active cobalt sites,which facilitated the formation of more C5+hydrocarbons.This study provides a promising method for support modification with incorporatedheteroatoms for the rational development of Fischer–Tropsch catalysts.展开更多
基金funding support from the National Natural Science Foundation of China (51722404, 51674177, 91845113 and 51804221)the “1000-Youth Talents Plan”+3 种基金the Fundamental Research Funds for the Central Universities (2042017kf0200)National Key R&D Program of China (2018YFE0201703)the China Postdoctoral Science Foundation (2018M642906 and 2019T120684)Hubei Provincial Natural Science Foundation of China (2019CFA065)。
文摘Structural and compositional design of core-shell structure is an effective strategy towards enhanced catalysis.Herein,amorphous MnO2 nanosheets and K+-intercalated layered MnO2 nanosheets are controllably assembled over Fe2O3 spindles,in which the MnO2 nanosheets are perpendicularly anchored to the surface of Fe2O3.Such a core shell structure contributes to a high specific surface area and abundant pore channels on the surface of catalysts.In addition,the existence of K+provides large numbers of basic sites and restrains the formation of unpleasant(Fe1-xMnx)3O4.Benefiting from the merits in structure and composition,CO adsorption is enhanced and remaining time of intermediates is prolonged on the surfaces of catalysts during the Fischer–Tropsch synthesis(FTS),facilitating to the formation of active iron carbides and C–C coupling reactions.Resultantly,the Fe2O3@K+-Mn O2 shows both a high CO conversion of 82.3%and a high C5+ selectivity of 73.1%.The present study provides structural and compositional rationales on design high-performance catalysts towards FTS.
文摘Single-wall carbon nanotubes （SWNTs） with high surface area were synthesized over nanoporous Co-Mo/MgO by a chemical vapor deposition （CVD） method. The SWNTs were used as catalyst support for selective hydrogenation of syngas to hydrocarbons. Here an extensive study of Fischer-Tropsch synthesis （FTS） on CNT-supported cobalt catalysts with different amounts of cobalt loading up to 40 wt% is reported. The catalysts were characterized by different methods including N2 adsorption-desorption, X-ray diffraction, hydrogen chemisorption, inductively coupled plasma （ICP） and temperature-programmed reduction. Enhancement of the reducibility of Co3O4 to CoO, CoO to Co° and small cobalt oxide particles, dispersion of the cobalt, and activity and selectivity of FTS were investigated and compared with a conventional support. The CNT supported catalysts achieve a high dispersion and high loading of the active metal, cobalt in particular, so that the bulk formation of cobalt metal, which tends to occur in conventional support, can be avoided. The results showed that the specific activity of CNT supported catalysts increase significantly （there is a two fold increase in CO Conversion per gram of the active metal） with respect to the conventional supported catalyst.
文摘The effect of reduction procedure on catalyst properties, activity and products selectivity of ruthenium-promoted Co/γ-Al2O3 catalyst in Fischer-Tropsch synthesis （FTS） was investigated. Catalyst samples were reduced with different reduction gas compositions and passivated before being characterized by TPR and XRD techniques. Different activity and product selectivity analyses were also performed. These results showed that the catalyst dispersion, particle size, and the degree of reduction changed with different reduction gas compositions, which were resulted from the water partial pressures in reduction process that give varying degrees of interaction with the support. It has been suggested that the FTS activity of cobalt catalyst was directly dependent on the catalyst reducibility. A reduction gas with a molar ratio of H2Prle = 1 was used to prevent the formation of Co-support compound during catalyst reduction.
基金support from the National Natural Science Foundation of China(Grant No.22078243)and the Program of Introducing Talents of Discipline to Universities(Grant No.BP0618007).
文摘Ordered SBA-15 mesoporous silica with incorporated titanium was successfully synthesized via a onepot hydrothermal crystallization method.The characterization including powder X-ray diffraction,Brunauer–Emmett–Teller,transmission electron microscope,temperatureprogrammed reduction,temperature-programmed desorption,Fourier transform infrared and ultraviolet-visible-near infrared spectrometer was performed to explore the physical and chemical structures of both the supports and the catalysts.The results showed that titanium was successfully incorporated into the mesoporous silica framework with a limited amount of titanium(Si/Ti>20),and the mesoporous structure was retained.However,the increased titanium content inevitably resulted in the formation of anatase TiO2 particles on the support surface.The increased incorporated titanium strengthened the interactions between cobalt species and supports,which was favorable for the cobalt species dispersion,despite the limited cobalt oxide reducibility.The enhanced metalsupport interactions were beneficial for the CO/H2 ratio at the active cobalt sites,which facilitated the formation of more C5+hydrocarbons.This study provides a promising method for support modification with incorporatedheteroatoms for the rational development of Fischer–Tropsch catalysts.
