A series of P/HZSM-5 catalysts prepared by impregnation method were used for ethanol conversion to lower olefins. The catalysts were characterized by X-ray diffraction (XRD), NH3-temperature-programmed desorption (...A series of P/HZSM-5 catalysts prepared by impregnation method were used for ethanol conversion to lower olefins. The catalysts were characterized by X-ray diffraction (XRD), NH3-temperature-programmed desorption (NH3-TPD) and N2 adsorption-desorption measurements. It was found that the P/HZSM-5 catalysts showed high activity and selectivity toward light olefins. The selectivities of propylene and butylene can be improved with the introduction of phosphorus (P). When the content of P reached 3.0 wt%, more than 18.9% propylene in the gaseous products was obtained over the P/HZSM-5 catalyst at 450 ?C. The introduction of P modified the strong Br?nsted acid sites of the original HZSM-5 catalysts and P/HZSM-5 catalysts could resist coke formation and showed good stability.展开更多
A series of Fe/HZSM-5 catalysts with different iron loadings were prepared by impregnation method.Characterization was performed by N2 adsorption-desorption,X-ray diffraction(XRD),NH3 temperature-programmed desorpt...A series of Fe/HZSM-5 catalysts with different iron loadings were prepared by impregnation method.Characterization was performed by N2 adsorption-desorption,X-ray diffraction(XRD),NH3 temperature-programmed desorption(NH3-TPD),temperature-programmed reduction (TPR),temperature-programmed oxidation(TPO)and thermogravimetry(TG)analysis.Iron content in the synthesized samples varied from 1.1 wt%to 20 wt%.The obtained samples have been used for ethanol conversion into light olefins.It was found that the amount of strong acidity at 300 -5 50-C on Fe-modified samples was decreased,going with another new acid site appearance at 550- 600-C and that Fe/HZSM-5 catalysts were highly selective towards light olefins,especially the 9FZ sample.In addition,Fe-modified catalysts suppressed the conversion of ethanol to aromatics and paraffins and enhanced their anti-carbon deposit ability.展开更多
Due to their environmentally friendly nature and high energy density,direct ethanol fuel cells have attracted extensive research attention in recent decades.However,the actual Faraday efficiency of the ethanol oxidati...Due to their environmentally friendly nature and high energy density,direct ethanol fuel cells have attracted extensive research attention in recent decades.However,the actual Faraday efficiency of the ethanol oxidation reaction(EOR)is much lower than its theoretical value and the reaction kinetics of the EOR is sluggish due to insufficient active sites on the electrocatalyst surface.Pt/C is recognized as one of the most promising electrocatalysts for the EOR.Thus,the microscopic interfacial reaction mechanisms of the EOR on Pt/C were systematically studied in this work.In metal hydroxide solutions,hydrated alkali cations were found to bind with OH_(ad)through noncovalent interactions to form clusters and occupy the active sites on the Pt/C electrocatalyst surface,thus resulting in low Faraday efficiency and sluggish kinetics of the EOR.To reduce the negative effect of the noncovalent interactions on the EOR,a shield was made on the electrocatalyst surface using 4-trifluoromethylphenyl,resulting in twice the EOR catalytic reactivity of Pt/C.展开更多
A multi-layer mesoporous silicalite-1 membrane supported on commercially available porous alumina tubes was prepared by firstly dip-coating the tubes in silica colloid sol and then using a hydrothermal synthetic proce...A multi-layer mesoporous silicalite-1 membrane supported on commercially available porous alumina tubes was prepared by firstly dip-coating the tubes in silica colloid sol and then using a hydrothermal synthetic process.The mesoporous silicalite-1 membrane was further modified by grafting organosilane compounds with various alkyl chains length(C_nH_(2n+1)(CH_3)_2SiCl;n = 1,3,8,12 and 18).These hydrophobic silicalite-1 membranes containing silane coupling agents effectively removed ethanol from 3 wt.%,5 wt.%and 10 wt.%aqueous ethanol solutions by pervaporation over a temperature range of 303-323 K.The separation factor(a) of ethanol decreased as the ethanol content in the feed solution increased from 3%to 10%whereas the permeation flux(J) basically remained constant.Ethanol separation factors(a) of 7.90-22.24 with total fluxes(J) of 0.76-2.89 kg/(m^2h) were obtained by pervaporation at 3_3-323 K for ethanol feed composition of 3%-10%.展开更多
基金supported by the Doctor Fund of Science Research of Xinjiang University (Grant No. BS060101)the National Natural ScienceFoundation of China (Grant No. 20963010)
文摘A series of P/HZSM-5 catalysts prepared by impregnation method were used for ethanol conversion to lower olefins. The catalysts were characterized by X-ray diffraction (XRD), NH3-temperature-programmed desorption (NH3-TPD) and N2 adsorption-desorption measurements. It was found that the P/HZSM-5 catalysts showed high activity and selectivity toward light olefins. The selectivities of propylene and butylene can be improved with the introduction of phosphorus (P). When the content of P reached 3.0 wt%, more than 18.9% propylene in the gaseous products was obtained over the P/HZSM-5 catalyst at 450 ?C. The introduction of P modified the strong Br?nsted acid sites of the original HZSM-5 catalysts and P/HZSM-5 catalysts could resist coke formation and showed good stability.
基金supported by the National Natural Science Foundation of China(No.20963010)the Doctor Fund of Science Research(No.070267)
文摘A series of Fe/HZSM-5 catalysts with different iron loadings were prepared by impregnation method.Characterization was performed by N2 adsorption-desorption,X-ray diffraction(XRD),NH3 temperature-programmed desorption(NH3-TPD),temperature-programmed reduction (TPR),temperature-programmed oxidation(TPO)and thermogravimetry(TG)analysis.Iron content in the synthesized samples varied from 1.1 wt%to 20 wt%.The obtained samples have been used for ethanol conversion into light olefins.It was found that the amount of strong acidity at 300 -5 50-C on Fe-modified samples was decreased,going with another new acid site appearance at 550- 600-C and that Fe/HZSM-5 catalysts were highly selective towards light olefins,especially the 9FZ sample.In addition,Fe-modified catalysts suppressed the conversion of ethanol to aromatics and paraffins and enhanced their anti-carbon deposit ability.
基金National Key R&D Program of China under Grant,Grant/Award Number:2021YFC1910601National Natural Science Foundation of China,Grant/Award Number:52104402HBIS Group Co.,Ltd Key R&D Program under Grant,Grant/Award Numbers:20210032,HG2022111。
文摘Due to their environmentally friendly nature and high energy density,direct ethanol fuel cells have attracted extensive research attention in recent decades.However,the actual Faraday efficiency of the ethanol oxidation reaction(EOR)is much lower than its theoretical value and the reaction kinetics of the EOR is sluggish due to insufficient active sites on the electrocatalyst surface.Pt/C is recognized as one of the most promising electrocatalysts for the EOR.Thus,the microscopic interfacial reaction mechanisms of the EOR on Pt/C were systematically studied in this work.In metal hydroxide solutions,hydrated alkali cations were found to bind with OH_(ad)through noncovalent interactions to form clusters and occupy the active sites on the Pt/C electrocatalyst surface,thus resulting in low Faraday efficiency and sluggish kinetics of the EOR.To reduce the negative effect of the noncovalent interactions on the EOR,a shield was made on the electrocatalyst surface using 4-trifluoromethylphenyl,resulting in twice the EOR catalytic reactivity of Pt/C.
基金the National Natural Science Foundation of China under Grant No.50972103the Scientific Research Foundation for Returned Overseas Chinese Scholars,Ministry of Education of China
文摘A multi-layer mesoporous silicalite-1 membrane supported on commercially available porous alumina tubes was prepared by firstly dip-coating the tubes in silica colloid sol and then using a hydrothermal synthetic process.The mesoporous silicalite-1 membrane was further modified by grafting organosilane compounds with various alkyl chains length(C_nH_(2n+1)(CH_3)_2SiCl;n = 1,3,8,12 and 18).These hydrophobic silicalite-1 membranes containing silane coupling agents effectively removed ethanol from 3 wt.%,5 wt.%and 10 wt.%aqueous ethanol solutions by pervaporation over a temperature range of 303-323 K.The separation factor(a) of ethanol decreased as the ethanol content in the feed solution increased from 3%to 10%whereas the permeation flux(J) basically remained constant.Ethanol separation factors(a) of 7.90-22.24 with total fluxes(J) of 0.76-2.89 kg/(m^2h) were obtained by pervaporation at 3_3-323 K for ethanol feed composition of 3%-10%.