The aim of this work was to evaluate the catalytic properties of a Ru promoted Co/SBA-15 catalyst for Fischer-Tropsch synthesis (FTS). The Ru promoted Co/SBA-15 catalyst was prepared by wet impregnation method and w...The aim of this work was to evaluate the catalytic properties of a Ru promoted Co/SBA-15 catalyst for Fischer-Tropsch synthesis (FTS). The Ru promoted Co/SBA-15 catalyst was prepared by wet impregnation method and was characterized by X-ray diffraction, X-ray energy dispersion spectrophotometer, N2 adsorption-desorption, temperature-programmed reduction and transmission electron microscopy. The Fischer-Tropsch synthesis using the catalyst was carried out to evaluate the catalyst activity and its effect on FTS product distribution. The synthesis was carried out in a slurry reactor operating at 513 K, 20 atm, CO : H2 molar ratio of 1 : 1. X-ray diffraction showed that the calcined cobalt catalyst did not modify the structure of SBA-15, proving that Co was present in the form of Co3O4 in the catalyst. The addition of cobalt in SBA-15 decreased the specific superficial area of the molecular sieve. Fischer-Tropsch synthesis activity and C5+ hydrocarbon selectivity increased with the addition of Ru. The increases in activity and selectivity were attributed to the increased number of active sites resulting from higher reducibility and the synergetic effect of Ru and Co. Ru/Co/SBA-15 catalysts showed moderate conversion (40%) and high selectivity towards the production of C5+ (80 wt%).展开更多
Dielectric barrier discharge(DBD)plasma excited by a high-frequency alternating-current(AC)power supply is widely employed for the degradation of volatile organic compounds(VOCs).However,the thermal effect generated d...Dielectric barrier discharge(DBD)plasma excited by a high-frequency alternating-current(AC)power supply is widely employed for the degradation of volatile organic compounds(VOCs).However,the thermal effect generated during the discharge process leads to energy waste and low energy utilization efficiency.In this work,an innovative DBD thermally-conducted catalysis(DBD-TCC)system,integrating high-frequency AC-DBD plasma and its generated thermal effects to activate the Co/SBA-15 catalyst,was employed for toluene removal.Specifically,Co/SBA-15 catalysts are closely positioned to the ground electrode of the plasma zone and can be heated and activated by the thermal effect when the voltage exceeds 10 k V.At12.4 k V,the temperature in the catalyst zone reached 261℃ in the DBD-TCC system,resulting in an increase in toluene degradation efficiency of 17%,CO_(2)selectivity of 21.2%,and energy efficiency of 27%,respectively,compared to the DBD system alone.In contrast,the DBD thermally-unconducted catalysis(DBD-TUC)system fails to enhance toluene degradation due to insufficient heat absorption and catalytic activation,highlighting the crucial role of AC-DBD generated heat in the activation of the catalyst.Furthermore,the degradation pathway and mechanism of toluene in the DBD-TCC system were hypothesized.This work is expected to provide an energy-efficient approach for high-frequency AC-DBD plasma removal of VOCs.展开更多
A series of Ni/SBA-15 catalysts with Ni contents ranging from 5wt% to 20wt% as well as 10wt%Ni/10wt%CexZr1-xO2/SBA-15 (x=0, 0.5, 1) were prepared. The structures of the catalysts were characterized using XRD, TPR, T...A series of Ni/SBA-15 catalysts with Ni contents ranging from 5wt% to 20wt% as well as 10wt%Ni/10wt%CexZr1-xO2/SBA-15 (x=0, 0.5, 1) were prepared. The structures of the catalysts were characterized using XRD, TPR, TEM and BET techniques. The catalytic activities of the catalysts for steam reforming of methane were evaluated in a continuous flow microreactor. The results indicated that both the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts had good catalytic activities at at- mospheric pressure. The 10wt%Ni/SBA-15 catalyst exhibited excellent stability at 800 ℃ for time on stream of 740 h. After the reaction, carbon deposits were not formed on the surface of the catalyst. There existed a regular hexagonal mesoporous structure in the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts. The nickel species and the CexZr1-xO2 component were all confined in the SBA-15 mesopores. The CexZr1-xO2 could promote dispersion of the nickel species in the Ni/CexZr1-xO2/SBA-15 catalysts.展开更多
A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray phot...A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray photoelectron spectroscopy (XPS) and H2-temperature programmed reduction. Their performances in long chain alkane dehydrogenation were evaluated in a fixed-bed microreactor with dodecane as a model alkane. The results indicated that SBA-15 maintained the well-order mesoporous structure during the reaction. The performance of the catalyst was found not dominated by its textural properties, but by the molar ratio of Sn to Pt which governed the degree of Sn reduction. Owing to the highest degree of Sn reduction, 1% (by mass) Pt-1.8% (by mass) Sn/SBA-15 showed the best catalytic activity. At 0.1 MPa and 470℃, the molar ratio of hydrogen to alkane at 4, and liquid hourly space velocity (LHSV) 20 h^-1, the dodecane conversion is 10%, and the dodecene selectivity is about 70%.展开更多
A new method for the preparation of SBA-15-supported palladium catalyst for Heck reaction in supercritical carbon dioxide was presented.The newly formed SBA-15-supported palladium catalyst(Ph-SBA-15-PPh_3-Pd) exhibi...A new method for the preparation of SBA-15-supported palladium catalyst for Heck reaction in supercritical carbon dioxide was presented.The newly formed SBA-15-supported palladium catalyst(Ph-SBA-15-PPh_3-Pd) exhibited high catalytic activity for the Heck reaction of 4-nitrobromobenzene with methyl acrylate.The catalyst can be reused several times without a loss of activity.展开更多
A series of Ni/SBA-15 catalysts with 5wt% to 15wt% Ni content as well as a series of 12.5%Ni/Cu/SBA-15 catalysts with 1% to 10% copper content were prepared by the impregnation method. The catalytic performance for pa...A series of Ni/SBA-15 catalysts with 5wt% to 15wt% Ni content as well as a series of 12.5%Ni/Cu/SBA-15 catalysts with 1% to 10% copper content were prepared by the impregnation method. The catalytic performance for partial oxidation of methane was investigated in a continuous flow microreactor under atmospheric pressure. The textural and chemical properties of the catalysts were characterized by XRD, TEM, BET and Hz-TPR techniques. The results indicated that the catalysts modified with Cu promoter showed better performance than those without modification. For the 12.5%Ni/2.5%/Cu/SBA-15 catalyst, at 850 ℃ the conversion of CH4 reached 97.9% and the selectivity of CO and H2 reached 98.0% and 96.0%, respectively. In XRD patterns of the Ni/Cu/SBA-15 catalyst with 7.5 to 10% Cu contents there were CuO characteristic peaks beside NiO characteristic peaks. The mesoporous structure of SBA-15 was retained in all of the catalysts. TPR analysis of the catalysts revealed that a strong interaction between Ni, Cu promoter and SBA-15 support may be existed. This interaction enhanced significantly the redox properties of the catalysts resulting in the higher catalytic activity.展开更多
基金supported by the Coordenao de Aperfeioamento de Pessoal de Nível Superior(CAPES)and Petrobras
文摘The aim of this work was to evaluate the catalytic properties of a Ru promoted Co/SBA-15 catalyst for Fischer-Tropsch synthesis (FTS). The Ru promoted Co/SBA-15 catalyst was prepared by wet impregnation method and was characterized by X-ray diffraction, X-ray energy dispersion spectrophotometer, N2 adsorption-desorption, temperature-programmed reduction and transmission electron microscopy. The Fischer-Tropsch synthesis using the catalyst was carried out to evaluate the catalyst activity and its effect on FTS product distribution. The synthesis was carried out in a slurry reactor operating at 513 K, 20 atm, CO : H2 molar ratio of 1 : 1. X-ray diffraction showed that the calcined cobalt catalyst did not modify the structure of SBA-15, proving that Co was present in the form of Co3O4 in the catalyst. The addition of cobalt in SBA-15 decreased the specific superficial area of the molecular sieve. Fischer-Tropsch synthesis activity and C5+ hydrocarbon selectivity increased with the addition of Ru. The increases in activity and selectivity were attributed to the increased number of active sites resulting from higher reducibility and the synergetic effect of Ru and Co. Ru/Co/SBA-15 catalysts showed moderate conversion (40%) and high selectivity towards the production of C5+ (80 wt%).
基金supported by National Natural Science Foundation of China(No.52177130)the Key Projects for Industrial Prospects and Core Technology Research in Suzhou City(No.SYC2022029)。
文摘Dielectric barrier discharge(DBD)plasma excited by a high-frequency alternating-current(AC)power supply is widely employed for the degradation of volatile organic compounds(VOCs).However,the thermal effect generated during the discharge process leads to energy waste and low energy utilization efficiency.In this work,an innovative DBD thermally-conducted catalysis(DBD-TCC)system,integrating high-frequency AC-DBD plasma and its generated thermal effects to activate the Co/SBA-15 catalyst,was employed for toluene removal.Specifically,Co/SBA-15 catalysts are closely positioned to the ground electrode of the plasma zone and can be heated and activated by the thermal effect when the voltage exceeds 10 k V.At12.4 k V,the temperature in the catalyst zone reached 261℃ in the DBD-TCC system,resulting in an increase in toluene degradation efficiency of 17%,CO_(2)selectivity of 21.2%,and energy efficiency of 27%,respectively,compared to the DBD system alone.In contrast,the DBD thermally-unconducted catalysis(DBD-TUC)system fails to enhance toluene degradation due to insufficient heat absorption and catalytic activation,highlighting the crucial role of AC-DBD generated heat in the activation of the catalyst.Furthermore,the degradation pathway and mechanism of toluene in the DBD-TCC system were hypothesized.This work is expected to provide an energy-efficient approach for high-frequency AC-DBD plasma removal of VOCs.
基金Financial funds from the Chinese Natural Science Foundation(Project No.20473009)the Beijing Natural Science Foundation(Project No.8062023)+1 种基金the National Basic Research Program of China(Project No.2005CB221405)the National"863"Project of China(No.2006 AA10Z425)are gratefully acknowledged.
文摘A series of Ni/SBA-15 catalysts with Ni contents ranging from 5wt% to 20wt% as well as 10wt%Ni/10wt%CexZr1-xO2/SBA-15 (x=0, 0.5, 1) were prepared. The structures of the catalysts were characterized using XRD, TPR, TEM and BET techniques. The catalytic activities of the catalysts for steam reforming of methane were evaluated in a continuous flow microreactor. The results indicated that both the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts had good catalytic activities at at- mospheric pressure. The 10wt%Ni/SBA-15 catalyst exhibited excellent stability at 800 ℃ for time on stream of 740 h. After the reaction, carbon deposits were not formed on the surface of the catalyst. There existed a regular hexagonal mesoporous structure in the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts. The nickel species and the CexZr1-xO2 component were all confined in the SBA-15 mesopores. The CexZr1-xO2 could promote dispersion of the nickel species in the Ni/CexZr1-xO2/SBA-15 catalysts.
基金Supported by the National Natural Science Foundation of China (20376005).
文摘A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray photoelectron spectroscopy (XPS) and H2-temperature programmed reduction. Their performances in long chain alkane dehydrogenation were evaluated in a fixed-bed microreactor with dodecane as a model alkane. The results indicated that SBA-15 maintained the well-order mesoporous structure during the reaction. The performance of the catalyst was found not dominated by its textural properties, but by the molar ratio of Sn to Pt which governed the degree of Sn reduction. Owing to the highest degree of Sn reduction, 1% (by mass) Pt-1.8% (by mass) Sn/SBA-15 showed the best catalytic activity. At 0.1 MPa and 470℃, the molar ratio of hydrogen to alkane at 4, and liquid hourly space velocity (LHSV) 20 h^-1, the dodecane conversion is 10%, and the dodecene selectivity is about 70%.
基金National Natural Science Foundation of China(No.20603005)the Specialized Research Fund for the Doctoral Program of Higher Education(No.20090041110012) for their financial support
文摘A new method for the preparation of SBA-15-supported palladium catalyst for Heck reaction in supercritical carbon dioxide was presented.The newly formed SBA-15-supported palladium catalyst(Ph-SBA-15-PPh_3-Pd) exhibited high catalytic activity for the Heck reaction of 4-nitrobromobenzene with methyl acrylate.The catalyst can be reused several times without a loss of activity.
基金supported by the National Basic Research Program of China (Project No. 2005CB221405)the National "863" Project of China (No.2006AA10Z425)
文摘A series of Ni/SBA-15 catalysts with 5wt% to 15wt% Ni content as well as a series of 12.5%Ni/Cu/SBA-15 catalysts with 1% to 10% copper content were prepared by the impregnation method. The catalytic performance for partial oxidation of methane was investigated in a continuous flow microreactor under atmospheric pressure. The textural and chemical properties of the catalysts were characterized by XRD, TEM, BET and Hz-TPR techniques. The results indicated that the catalysts modified with Cu promoter showed better performance than those without modification. For the 12.5%Ni/2.5%/Cu/SBA-15 catalyst, at 850 ℃ the conversion of CH4 reached 97.9% and the selectivity of CO and H2 reached 98.0% and 96.0%, respectively. In XRD patterns of the Ni/Cu/SBA-15 catalyst with 7.5 to 10% Cu contents there were CuO characteristic peaks beside NiO characteristic peaks. The mesoporous structure of SBA-15 was retained in all of the catalysts. TPR analysis of the catalysts revealed that a strong interaction between Ni, Cu promoter and SBA-15 support may be existed. This interaction enhanced significantly the redox properties of the catalysts resulting in the higher catalytic activity.