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
PtSnNa/AlSBA-15 catalysts with different amounts of Sn were prepared for propane dehydrogenation.The catalysts were characterized by XRF,BET,H2 chemisorption,NH3-TPD,H2-TPR,and TPO techniques.Test results indicated th...PtSnNa/AlSBA-15 catalysts with different amounts of Sn were prepared for propane dehydrogenation.The catalysts were characterized by XRF,BET,H2 chemisorption,NH3-TPD,H2-TPR,and TPO techniques.Test results indicated that the presence of tin not only modified the acid function and the interfacial character between metal and support,but also reduced the coke deposition effectively.Among these catalysts investigated thereby,the PtSn(0.7%)Na/AlSBA-15 catalyst had the best catalytic performance in terms of propane conversion and stability.With the continuous addition of Sn,more amounts of Sn0 species appeared,which was unfavorable to the reaction.The PtSn(0.7%)Na/AlSBA-15 catalyst was parametrically characterized in order to obtain necessary information to integrate the process operating conditions.A weight hourly space velocity of 3 h-1,a reaction temperature of 610 ℃ and a H2/C3H8 molar ratio of 0.25 were found to be optimum conditions for achieving a higher dehydrogenation activity of the catalyst.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 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
A series of Ni/SBA-15 catalysts with Ni contents ranging from 5 wt% to 15 wt%, as well as another series of 10%Ni/MgO/SBA-15 catalysts, in which the range of the MgO content was from 1 wt% to 7 wt%, were prepared, and...A series of Ni/SBA-15 catalysts with Ni contents ranging from 5 wt% to 15 wt%, as well as another series of 10%Ni/MgO/SBA-15 catalysts, in which the range of the MgO content was from 1 wt% to 7 wt%, were prepared, and their catalytic performances for the reaction of combined steam and carbon dioxide reforming of methane were investigated in a continuous flow microreactor. The structures of the catalysts were characterized using the XRD, H2-TPR and CO2-TPD techniques. The results indicated that the CO selectivity for this reaction was very close to 100%, and the H2/CO ratio of the product gas could be controlled by changing the H2O/CO2 molar ratio of the feed gas. The simultaneous and plentiful existing of steam and CO2 had a significant influence on the catalytic performance of the 10%Ni/SBA-15 catalyst without modification. After reacting at 850 °C for 120 h over this catalyst, the CH4 conversion dropped from 98% to 85%, and the CO2 conversion decreased from 86% to 53%. However, the 10%Ni/3%MgO/SBA-15 catalyst exhibited a much better catalytic performance, and after reacting for 620 h, the CO2 conversion over this catalyst dropped from 92% to around 77%, while the CH4 conversion was not decreased. Oxidation of the Ni0 species as well as carbon deposition during the reaction were the main reasons for the deactivation of the catalyst without modification. On the other hand, modification by the MgO promoter improved the dispersion of the Ni0 species, and enhanced the CO2 adsorption affinity which in turn depressed the occurring of carbon deposition, and thus retarded the deactivation process.展开更多
A series of Ni/SBA-15 catalysts with Ni contents from 7.5 wt% to 15 wt% were prepared by impregnation method.The effect of O2 and H2O on the combined reforming of the simulated biogas to syngas was investigated in a c...A series of Ni/SBA-15 catalysts with Ni contents from 7.5 wt% to 15 wt% were prepared by impregnation method.The effect of O2 and H2O on the combined reforming of the simulated biogas to syngas was investigated in a continuous flow fixed-bed micro-reactor.The stability of the catalyst was tested at 800 ？C.The results indicated that 10wt%Ni/SBA-15 catalyst exhibited the highest catalytic activities for the combined reforming of the simulated biogas to syngas.Under the reaction conditions of the feed gas molar ratios CH4/CO2/O2/H2O = 2/1/0.6/0.6,GHSV = 24000 ml·gcat^-1·h^-1 and the reaction temperature T = 800 ℃,the conversions of CH4 and CO2 were 92.8% and 76.3%,respectively,and the yields of CO and H2 were 99.0% and 82.0%,respectively.The catalytic activities of the catalyst did not decrease obviously after 100 h reaction time on stream.展开更多
Rod-like, hexagonal and fiber-like SBA-15 mesoporous silicas were synthesized to support MnO_x for toluene oxidation. This study showed that the morphology of the supports greatly influenced the catalytic activity in ...Rod-like, hexagonal and fiber-like SBA-15 mesoporous silicas were synthesized to support MnO_x for toluene oxidation. This study showed that the morphology of the supports greatly influenced the catalytic activity in toluene oxidation. MnO_x supported on rod-like SBA-15(R-SBA-15) displayed the best catalytic activity and the conversion at 230°C reached more than 90%, which was higher than the other two catalysts. MnO_x species consisted of coexisting MnO_2 and Mn_2O_3 on the three kinds of SBA-15 samples. Large amounts of Mn_2O_3 species were formed on the surface and high oxygen mobility was obtained on MnO_x supported on R-SBA-15, according to the H_2 temperature programmed reduction(H_2-TPR)and X-ray photoelectron spectroscopy(XPS) results. The Mn/R-SBA-15 catalyst with greater amounts of Mn_2O_3 species possessed a large amount of surface lattice oxygen, which accelerated the catalytic reaction rate. Therefore, the surface lattice oxygen and high oxygen mobility were critical factors on the catalytic activity of the Mn/R-SBA-15 catalyst.展开更多
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
The alumina-modified SBA-15 （A12OJSBA-15） zeolite was prepared in a non-aqueous system by using toluene as the solvent, and was used to support the PtSn-based catalyst for propane dehydrogenation. The BET surface ar...The alumina-modified SBA-15 （A12OJSBA-15） zeolite was prepared in a non-aqueous system by using toluene as the solvent, and was used to support the PtSn-based catalyst for propane dehydrogenation. The BET surface area mea- surements, hydrogen chemisorption, FT-IR spectroscopy, NH3-TPD, XPS and TPO techniques were used to characterize the catalysts. Test results showed that the addition of alumina not only could modify the acid function of the support but also the structure of the metallic phase, thus affecting their catalytic properties. Among these catalysts studied, the PtSn/AI203 （5%）/ SBA-15 catalyst exhibited a best catalytic performance in terms of propane conversion and selectivity to propene. The high catalytic performance might be attributed to the relatively good Pt metal dispersion and/or the strong interaction between Pt and Sn species.展开更多
The catalytic oxidation of toluene over Ag/SBA‐15synthesized under different pretreatment conditions,including O2at500°C(denoted O500),H2at500°C(H500),and O2at500°C followed by H2at300°C(O500‐H30...The catalytic oxidation of toluene over Ag/SBA‐15synthesized under different pretreatment conditions,including O2at500°C(denoted O500),H2at500°C(H500),and O2at500°C followed by H2at300°C(O500‐H300)was studied.The pretreated samples were investigated by N2physisorption,X‐ray diffraction,and ultraviolet‐visible diffuse reflectance.The pretreatment atmosphere greatly influences the status of the Ag and O species,which in turn significantly impacts the adsorption and catalytic removal of toluene.Ag2O and amorphous Ag particles,as well as a large amount of subsurface oxygen species,are formed on O500,and the subsurface oxygen enhances the interaction between Ag species and toluene,so O500shows good activity at higher temperature.However,its activity at lower temperature is not as high as expected,with a reduced presence of Ag2O and lower adsorption capacity for toluene.H2pretreatment at500°C is conducive to the formation of large Ag particles and yields the largest adsorption capacity for toluene,so H500exhibits the best activity at lower temperatures;however,because of poor interaction between Ag and toluene,its activity at higher temperature is modest.The O500‐H300sample exhibits excellent catalytic activity during the whole reaction process,which can be attributed to the small and highly dispersed Ag nanoparticles as well as the existence of subsurface oxygen.展开更多
The Al-doped Ni2P/AI-SBA-15 catalyst with high hydrodeoxygenation （HDO） activity was synthesized by tem- perature programmed reduction at a relatively low reduction temperature of 400 ℃. The as-prepared catalyst wa...The Al-doped Ni2P/AI-SBA-15 catalyst with high hydrodeoxygenation （HDO） activity was synthesized by tem- perature programmed reduction at a relatively low reduction temperature of 400 ℃. The as-prepared catalyst was characterized by X-ray diffraction （XRD）, H2 temperature-programmed reduction （H2-TPR）, X-ray photoelectron spectroscopy （XPS）, transmission electron microscope （TEM）, NH3 temperature programmed desorption （NH3-TPD）, N2 adsorption-desorption and CO uptake. The effect of AI on benzofuran （BF） HDO performance was investigated. The result indicates that the incorporation of AI into the SBA-15 support can promote the formation of much uniform, smaller, highly dispersed N2P particles on the catalyst. The AI also contrib- utes to suppress the enrichment of P and promote more exposed Ni sites on the surface. In addition, the incorporation of AI can enhance the acid strength. The total deoxygenated product yield over Ni2P/AI-SBA-15 reached 90.3%, which is an increase of 19.4%, when compared with that found for Ni2P/SBA-15 （70.9%）.展开更多
Efficiency and recycling of catalysts are important for the lignin hydrogenolysis to obtain phenolic monomers.In this work,a series of highdispersion Ni/AlSBA15 catalysts were prepared by a direct and effective prepar...Efficiency and recycling of catalysts are important for the lignin hydrogenolysis to obtain phenolic monomers.In this work,a series of highdispersion Ni/AlSBA15 catalysts were prepared by a direct and effective preparation method,and then used in the hydrogenolysis of diphenyl ether(DE)and organosolv hydrolyzed lignin(OHL)for phenolic monomers.The universality of asmade catalysts in different solvents and cyclic performance were investigated.Results showed that the addition of ethylene glycol(EG)during the loading process of Ni promoted the dispersion of metal efficiently.High dispersion of Ni species could highly enhance the conversion of DE and the OHL which Ni/AlSBA15(1EG)exhibited the excellent catalytic performance.Decalin was found to be most effective solvent on the conversion of DE(99.16%).84.77%liquefaction ratio and 21.36%monomer yield were achieved,and no obvious char was observed after the depolymerization of OHL in ethanol solvent at 280℃for 4 h over the Ni/AlSBA15(1EG)catalyst.展开更多
A series of SBA-15 supported bimetallic Rh–Ni catalysts with different weight ratio of Rh/Ni in the range of 0–0.04 were prepared for carbon dioxide reforming of methane. The doping effect of Rh on catalytic activit...A series of SBA-15 supported bimetallic Rh–Ni catalysts with different weight ratio of Rh/Ni in the range of 0–0.04 were prepared for carbon dioxide reforming of methane. The doping effect of Rh on catalytic activity as well as carbon accumulation and removal over the catalysts was studied. The characterization results indicated that the addition of a small amount of Rh promoted the reducibility of Ni particles and decreased the Ni particle size. During the dry reforming reaction, the carbon deposition was originated from CH4 decomposition and CO disproportionation. The Rh–Ni catalyst with small metallic particle size inhibited the carbon formation and exhibited high efficiency in the removal of coke. In comparison with bare Ni-based catalyst, the Rh–Ni bimetallic catalysts showed high activity and stability in the dry reforming of methane.展开更多
Abstract： The present article compares the propane dehydrogenation performance of alumina binder-added PtSnNa/ A1SBA-15 catalysts prepared via three different procedures in comparison with the performance of a binder...Abstract： The present article compares the propane dehydrogenation performance of alumina binder-added PtSnNa/ A1SBA-15 catalysts prepared via three different procedures in comparison with the performance of a binder-free PtSnNa/ AISBA-15 catalyst. All these catalysts have been investigated by reaction tests and some physico-chemical characterizations such as BET, H2 chemisorption, catalytic grain crushing strength, NHa-TPD and TPO analyses. Test results showed that the addition of alumina binder could enhance the mechanical strength of catalyst evidently. Moreover, the different preparation procedures not only modified the characteristics of both acid and metal functions but also affected the coke deposition on the catalysts. Among these catalysts studied, the catalyst prepared by impregnation followed by the agglomeration of alumi- na binder had exhibited the highest catalytic activity and stability compared with other catalyst samples undergoing different preparation procedures. The possible reason may be attributed to the highest metallic dispersion and the strong interactions among Pt, Sn and the support.展开更多
Hydrogen production through steam reforming of ethanol (SRE) over Mg modified Co-based catalysts supported on mesoporous SBA-15 was studied herein to evaluate the catalytic activity and the behavior of coke deposition...Hydrogen production through steam reforming of ethanol (SRE) over Mg modified Co-based catalysts supported on mesoporous SBA-15 was studied herein to evaluate the catalytic activity and the behavior of coke deposition. The CoyMgx/SBA-15 catalysts are obtained according to the steps of consecutive impregnation of Mg (x = 5 and 10 wt%) to be incorporated on SBA-15 and then follow the loading of Co (y = 10 and 20 wt%) using the incipient wetness impregnation method. The catalysts are characterized by using X-ray diffraction (XRD), temperature programmed reduction (TPR), transmission electron microscopy (TEM) and BET techniques. Also, the spent catalysts are further characterized by using XRD and TEM. The catalytic activity of the SRE is evaluated in a fixed-bed reactor under 22,000 h-1 GHSV and with an H2O/EtOH molar ratio of 13. All the CoyMgx/SBA-15 catalysts present a mesoporous structure, even after the SRE reaction. The optimum catalyst of Co20Mg5/SBA-15-H650 comes from the high loading of Co and high reduction temperature pretreatment, which show a high catalytic activity and stability at 550°C with a hydrogen yield (YH2) up to 5.78 and CO selectivity around 3.10%.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 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
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the Production and Research Prospective Joint Research Project(BY2009153)the Science and Technology Support Program(BE2008129) of Jiangsu Province of Chinathe National Nature Science Foundation of China(50873026) for financial supports
文摘PtSnNa/AlSBA-15 catalysts with different amounts of Sn were prepared for propane dehydrogenation.The catalysts were characterized by XRF,BET,H2 chemisorption,NH3-TPD,H2-TPR,and TPO techniques.Test results indicated that the presence of tin not only modified the acid function and the interfacial character between metal and support,but also reduced the coke deposition effectively.Among these catalysts investigated thereby,the PtSn(0.7%)Na/AlSBA-15 catalyst had the best catalytic performance in terms of propane conversion and stability.With the continuous addition of Sn,more amounts of Sn0 species appeared,which was unfavorable to the reaction.The PtSn(0.7%)Na/AlSBA-15 catalyst was parametrically characterized in order to obtain necessary information to integrate the process operating conditions.A weight hourly space velocity of 3 h-1,a reaction temperature of 610 ℃ and a H2/C3H8 molar ratio of 0.25 were found to be optimum conditions for achieving a higher dehydrogenation activity of the catalyst.
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 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.
基金the National Basic Research Program ofChina (Project No. 2005CB221405)the National "863" Project ofChina (No. 2006AA10Z425)the Beijing Natural Science Foun-dation (Project No: 8062023)
文摘A series of Ni/SBA-15 catalysts with Ni contents ranging from 5 wt% to 15 wt%, as well as another series of 10%Ni/MgO/SBA-15 catalysts, in which the range of the MgO content was from 1 wt% to 7 wt%, were prepared, and their catalytic performances for the reaction of combined steam and carbon dioxide reforming of methane were investigated in a continuous flow microreactor. The structures of the catalysts were characterized using the XRD, H2-TPR and CO2-TPD techniques. The results indicated that the CO selectivity for this reaction was very close to 100%, and the H2/CO ratio of the product gas could be controlled by changing the H2O/CO2 molar ratio of the feed gas. The simultaneous and plentiful existing of steam and CO2 had a significant influence on the catalytic performance of the 10%Ni/SBA-15 catalyst without modification. After reacting at 850 °C for 120 h over this catalyst, the CH4 conversion dropped from 98% to 85%, and the CO2 conversion decreased from 86% to 53%. However, the 10%Ni/3%MgO/SBA-15 catalyst exhibited a much better catalytic performance, and after reacting for 620 h, the CO2 conversion over this catalyst dropped from 92% to around 77%, while the CH4 conversion was not decreased. Oxidation of the Ni0 species as well as carbon deposition during the reaction were the main reasons for the deactivation of the catalyst without modification. On the other hand, modification by the MgO promoter improved the dispersion of the Ni0 species, and enhanced the CO2 adsorption affinity which in turn depressed the occurring of carbon deposition, and thus retarded the deactivation process.
基金supported by the National Basic Research Program of China(Project No.2005CB221405)the National "863" Project of China (No.2006AA10Z425)the Beijing Natural Science Foundation (Project No: 8062023)
文摘A series of Ni/SBA-15 catalysts with Ni contents from 7.5 wt% to 15 wt% were prepared by impregnation method.The effect of O2 and H2O on the combined reforming of the simulated biogas to syngas was investigated in a continuous flow fixed-bed micro-reactor.The stability of the catalyst was tested at 800 ？C.The results indicated that 10wt%Ni/SBA-15 catalyst exhibited the highest catalytic activities for the combined reforming of the simulated biogas to syngas.Under the reaction conditions of the feed gas molar ratios CH4/CO2/O2/H2O = 2/1/0.6/0.6,GHSV = 24000 ml·gcat^-1·h^-1 and the reaction temperature T = 800 ℃,the conversions of CH4 and CO2 were 92.8% and 76.3%,respectively,and the yields of CO and H2 were 99.0% and 82.0%,respectively.The catalytic activities of the catalyst did not decrease obviously after 100 h reaction time on stream.
基金supported by the National Nature Science Foundation of China (Nos.21377016 and 21577014)Programme of Introducing Talents of Discipline to Universities (No.B13012)Program for Changjiang Scholars and Innovative Research Team in University (No.IRT_13R05)
文摘Rod-like, hexagonal and fiber-like SBA-15 mesoporous silicas were synthesized to support MnO_x for toluene oxidation. This study showed that the morphology of the supports greatly influenced the catalytic activity in toluene oxidation. MnO_x supported on rod-like SBA-15(R-SBA-15) displayed the best catalytic activity and the conversion at 230°C reached more than 90%, which was higher than the other two catalysts. MnO_x species consisted of coexisting MnO_2 and Mn_2O_3 on the three kinds of SBA-15 samples. Large amounts of Mn_2O_3 species were formed on the surface and high oxygen mobility was obtained on MnO_x supported on R-SBA-15, according to the H_2 temperature programmed reduction(H_2-TPR)and X-ray photoelectron spectroscopy(XPS) results. The Mn/R-SBA-15 catalyst with greater amounts of Mn_2O_3 species possessed a large amount of surface lattice oxygen, which accelerated the catalytic reaction rate. Therefore, the surface lattice oxygen and high oxygen mobility were critical factors on the catalytic activity of the Mn/R-SBA-15 catalyst.
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the National Nature Science Foundation of China (50873026, 21106017)the Production and Research Prospective Joint Research Project (BY2009153)+1 种基金the Science and Technology Support Program (BE2008129) of Jiangsu Province of Chinathe Specialized Research Fund for the Doctoral Program of Higher Education of China (20100092120047) for financial supports
文摘The alumina-modified SBA-15 （A12OJSBA-15） zeolite was prepared in a non-aqueous system by using toluene as the solvent, and was used to support the PtSn-based catalyst for propane dehydrogenation. The BET surface area mea- surements, hydrogen chemisorption, FT-IR spectroscopy, NH3-TPD, XPS and TPO techniques were used to characterize the catalysts. Test results showed that the addition of alumina not only could modify the acid function of the support but also the structure of the metallic phase, thus affecting their catalytic properties. Among these catalysts studied, the PtSn/AI203 （5%）/ SBA-15 catalyst exhibited a best catalytic performance in terms of propane conversion and selectivity to propene. The high catalytic performance might be attributed to the relatively good Pt metal dispersion and/or the strong interaction between Pt and Sn species.
基金supported by the National Natural Science Foundation of China(21377016,21577014)Program for Changjiang Scholars and Innovative Research Team in University(IRT_13R05)~~
文摘The catalytic oxidation of toluene over Ag/SBA‐15synthesized under different pretreatment conditions,including O2at500°C(denoted O500),H2at500°C(H500),and O2at500°C followed by H2at300°C(O500‐H300)was studied.The pretreated samples were investigated by N2physisorption,X‐ray diffraction,and ultraviolet‐visible diffuse reflectance.The pretreatment atmosphere greatly influences the status of the Ag and O species,which in turn significantly impacts the adsorption and catalytic removal of toluene.Ag2O and amorphous Ag particles,as well as a large amount of subsurface oxygen species,are formed on O500,and the subsurface oxygen enhances the interaction between Ag species and toluene,so O500shows good activity at higher temperature.However,its activity at lower temperature is not as high as expected,with a reduced presence of Ag2O and lower adsorption capacity for toluene.H2pretreatment at500°C is conducive to the formation of large Ag particles and yields the largest adsorption capacity for toluene,so H500exhibits the best activity at lower temperatures;however,because of poor interaction between Ag and toluene,its activity at higher temperature is modest.The O500‐H300sample exhibits excellent catalytic activity during the whole reaction process,which can be attributed to the small and highly dispersed Ag nanoparticles as well as the existence of subsurface oxygen.
文摘The Al-doped Ni2P/AI-SBA-15 catalyst with high hydrodeoxygenation （HDO） activity was synthesized by tem- perature programmed reduction at a relatively low reduction temperature of 400 ℃. The as-prepared catalyst was characterized by X-ray diffraction （XRD）, H2 temperature-programmed reduction （H2-TPR）, X-ray photoelectron spectroscopy （XPS）, transmission electron microscope （TEM）, NH3 temperature programmed desorption （NH3-TPD）, N2 adsorption-desorption and CO uptake. The effect of AI on benzofuran （BF） HDO performance was investigated. The result indicates that the incorporation of AI into the SBA-15 support can promote the formation of much uniform, smaller, highly dispersed N2P particles on the catalyst. The AI also contrib- utes to suppress the enrichment of P and promote more exposed Ni sites on the surface. In addition, the incorporation of AI can enhance the acid strength. The total deoxygenated product yield over Ni2P/AI-SBA-15 reached 90.3%, which is an increase of 19.4%, when compared with that found for Ni2P/SBA-15 （70.9%）.
基金the National Natural Science Foundation of China(No.51676191&5181101221)Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01N092)+1 种基金“Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA 21060102)Jiangsu Key Laboratory for Biomass Energy and Material(JSBEM201905).
文摘Efficiency and recycling of catalysts are important for the lignin hydrogenolysis to obtain phenolic monomers.In this work,a series of highdispersion Ni/AlSBA15 catalysts were prepared by a direct and effective preparation method,and then used in the hydrogenolysis of diphenyl ether(DE)and organosolv hydrolyzed lignin(OHL)for phenolic monomers.The universality of asmade catalysts in different solvents and cyclic performance were investigated.Results showed that the addition of ethylene glycol(EG)during the loading process of Ni promoted the dispersion of metal efficiently.High dispersion of Ni species could highly enhance the conversion of DE and the OHL which Ni/AlSBA15(1EG)exhibited the excellent catalytic performance.Decalin was found to be most effective solvent on the conversion of DE(99.16%).84.77%liquefaction ratio and 21.36%monomer yield were achieved,and no obvious char was observed after the depolymerization of OHL in ethanol solvent at 280℃for 4 h over the Ni/AlSBA15(1EG)catalyst.
基金supported by the National Natural Science Foundation of China(21173050,21371035)
文摘A series of SBA-15 supported bimetallic Rh–Ni catalysts with different weight ratio of Rh/Ni in the range of 0–0.04 were prepared for carbon dioxide reforming of methane. The doping effect of Rh on catalytic activity as well as carbon accumulation and removal over the catalysts was studied. The characterization results indicated that the addition of a small amount of Rh promoted the reducibility of Ni particles and decreased the Ni particle size. During the dry reforming reaction, the carbon deposition was originated from CH4 decomposition and CO disproportionation. The Rh–Ni catalyst with small metallic particle size inhibited the carbon formation and exhibited high efficiency in the removal of coke. In comparison with bare Ni-based catalyst, the Rh–Ni bimetallic catalysts showed high activity and stability in the dry reforming of methane.
基金the National Nature Science Foundation of China(50873026,and21106017)the Production and Research Prospective Joint Research Project(BY2009153)+1 种基金the Science and Technology Support Program(BE2008129) of Jiangsu Province of ChinaSpecialized Research Fund for the Doctoral Program of Higher Education of China(20100092120047) for financial supports
文摘Abstract： The present article compares the propane dehydrogenation performance of alumina binder-added PtSnNa/ A1SBA-15 catalysts prepared via three different procedures in comparison with the performance of a binder-free PtSnNa/ AISBA-15 catalyst. All these catalysts have been investigated by reaction tests and some physico-chemical characterizations such as BET, H2 chemisorption, catalytic grain crushing strength, NHa-TPD and TPO analyses. Test results showed that the addition of alumina binder could enhance the mechanical strength of catalyst evidently. Moreover, the different preparation procedures not only modified the characteristics of both acid and metal functions but also affected the coke deposition on the catalysts. Among these catalysts studied, the catalyst prepared by impregnation followed by the agglomeration of alumi- na binder had exhibited the highest catalytic activity and stability compared with other catalyst samples undergoing different preparation procedures. The possible reason may be attributed to the highest metallic dispersion and the strong interactions among Pt, Sn and the support.
文摘Hydrogen production through steam reforming of ethanol (SRE) over Mg modified Co-based catalysts supported on mesoporous SBA-15 was studied herein to evaluate the catalytic activity and the behavior of coke deposition. The CoyMgx/SBA-15 catalysts are obtained according to the steps of consecutive impregnation of Mg (x = 5 and 10 wt%) to be incorporated on SBA-15 and then follow the loading of Co (y = 10 and 20 wt%) using the incipient wetness impregnation method. The catalysts are characterized by using X-ray diffraction (XRD), temperature programmed reduction (TPR), transmission electron microscopy (TEM) and BET techniques. Also, the spent catalysts are further characterized by using XRD and TEM. The catalytic activity of the SRE is evaluated in a fixed-bed reactor under 22,000 h-1 GHSV and with an H2O/EtOH molar ratio of 13. All the CoyMgx/SBA-15 catalysts present a mesoporous structure, even after the SRE reaction. The optimum catalyst of Co20Mg5/SBA-15-H650 comes from the high loading of Co and high reduction temperature pretreatment, which show a high catalytic activity and stability at 550°C with a hydrogen yield (YH2) up to 5.78 and CO selectivity around 3.10%.
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.
