Introduced a method of synthesizing hierarchical EU-1 zeolite with organosilanes as additive, and studied the influences of following different kinds of organosilanes on the synthesis of hierarchical EU-1 zeolite: γ-...Introduced a method of synthesizing hierarchical EU-1 zeolite with organosilanes as additive, and studied the influences of following different kinds of organosilanes on the synthesis of hierarchical EU-1 zeolite: γ-glycidoxy propyl trimethoxy silane(GPTMS), N-β-(aminoethyl)-γ-aminopropyl methyl dimethoxyl silane(APAEDMS),and N-(β-aminoethyl)-γ-aminopropyl dimethoxyl(ethyoxyl) silane(TMPED). The hierarchical EU-1 samples were characterized by XRD, SEM, N_2 adsorption, FT-IR and NH_3-TPD to analyze the crystallinity, morphology, surface area, pore size distribution and acidity. The results showed that hierarchical EU-1 zeolites were successfully synthesized; organosilanes have great influence on crystal morphology of EU-1 zeolites; the exterior surface area of hierarchical EU-1 zeolite, which synthesized with organosilanes(APAEDMS) adding into synthesis system, increased by 62.1% and mesopore volume increased by 129.1% compared with conventional EU-1 zeolites, thus can reduce the diffusional restriction markedly in catalytic reaction. The catalytic performance of hierarchical EU-1zeolites were evaluated in m-xylene isomerization on fixed bed reactor. The catalytic data showed that the isomerization activity PX/X of the hierarchical EU-1 zeolites reached around 24.09% in theoretical thermodynamic equilibrium from 23.83%, and the selectivity of C_8 aromatic hydrocarbon increased from 75.16% to 84.87%. The conversion of p-xylene increased from 16.30% to 18.41%.展开更多
Desilication accompanied with minimum loss of crystallinity effect of a high alumina ZSM-5 zeolite on the isomerization reaction of ethylbenzene/xylene mixtures has been considered.Desilication was assessed through XR...Desilication accompanied with minimum loss of crystallinity effect of a high alumina ZSM-5 zeolite on the isomerization reaction of ethylbenzene/xylene mixtures has been considered.Desilication was assessed through XRF,XRD,FTIR,TEM,nitrogen adsorption/desorption,NH_3-TPD,^(29)Si and^(27)Al MAS NMR analytical techniques.Desilication was accompanied with the creation of super acid sites.There exists a limit(Si/Al molar ratio of9.67)for keeping high crystallinity and obtaining improved catalytic performance.Desilication promotes ethylbenzene conversion by disproportionation and trans-alkylation reactions while the same reactions are limited for the xylene isomers.The p-xylene approach to equilibrium improves by more than 7% at 400℃ and a WHSV of 2 h^(-1)for the optimum sample with respect to the parent zeolite.At the same conditions,the optimum sample exhibits the maximum ethylbenzene conversion of 89%,i.e.more than 40%w.r.t.of the parent zeolite.However,the xylene yield decreases only 3%.展开更多
MIL-125 is a metal-organic framework with great potential for the adsorption and separation of xylene isomers.However,MIL-125 is usually synthesized under anhydrous and anaerobic conditions.In this study,homogeneously...MIL-125 is a metal-organic framework with great potential for the adsorption and separation of xylene isomers.However,MIL-125 is usually synthesized under anhydrous and anaerobic conditions.In this study,homogeneously shaped and highly crystalline MIL-125 was synthesized by introducing water-resistant titanium-containing oligomers into the synthesis process.With the assistance of the novel oligomers,MIL-125 can be synthesized in the presence of water,which meets batch-production requirements.The adsorption separation performance of the obtained highly crystalline MIL-125 was also significantly enhanced.The para-xylene/meta-xylene selectivity can reach 13.5 in mesitylene,which is higher than the selectivity values of most previously reported para-selective adsorbents.The MIL-125 xylene separation performance was verified using both batch adsorption and breakthrough experiments in the liquid phase.In addition,the influence of the solvent effect was evaluated through microcalorimetric experiments,liquid-phase adsorption experiments,and theoretical calculations.展开更多
1. Introduction Zeolites are widely used in acid heterogeneous catalysis [1, 2]. Due to the unique physical and chemical properties ofzeolites, they are widely used in commercial catalytic processes, such as fluidized...1. Introduction Zeolites are widely used in acid heterogeneous catalysis [1, 2]. Due to the unique physical and chemical properties ofzeolites, they are widely used in commercial catalytic processes, such as fluidized catalytic cracking, hydrocracking, methanol conversion to gasoline or olefins, ethylbenzene production, xylene isomerization, aromatics hydrogenation [3-9]. Acidity, high thermal stability, and shape selectivity determine the use of zeolites as catalysts in reaction processes through acid mechanisms [ 10].展开更多
基金Supported by the National Innovation Fund for Small and Medium-sized Technology-based Firms(14C26211400552)
文摘Introduced a method of synthesizing hierarchical EU-1 zeolite with organosilanes as additive, and studied the influences of following different kinds of organosilanes on the synthesis of hierarchical EU-1 zeolite: γ-glycidoxy propyl trimethoxy silane(GPTMS), N-β-(aminoethyl)-γ-aminopropyl methyl dimethoxyl silane(APAEDMS),and N-(β-aminoethyl)-γ-aminopropyl dimethoxyl(ethyoxyl) silane(TMPED). The hierarchical EU-1 samples were characterized by XRD, SEM, N_2 adsorption, FT-IR and NH_3-TPD to analyze the crystallinity, morphology, surface area, pore size distribution and acidity. The results showed that hierarchical EU-1 zeolites were successfully synthesized; organosilanes have great influence on crystal morphology of EU-1 zeolites; the exterior surface area of hierarchical EU-1 zeolite, which synthesized with organosilanes(APAEDMS) adding into synthesis system, increased by 62.1% and mesopore volume increased by 129.1% compared with conventional EU-1 zeolites, thus can reduce the diffusional restriction markedly in catalytic reaction. The catalytic performance of hierarchical EU-1zeolites were evaluated in m-xylene isomerization on fixed bed reactor. The catalytic data showed that the isomerization activity PX/X of the hierarchical EU-1 zeolites reached around 24.09% in theoretical thermodynamic equilibrium from 23.83%, and the selectivity of C_8 aromatic hydrocarbon increased from 75.16% to 84.87%. The conversion of p-xylene increased from 16.30% to 18.41%.
基金financed by BIPC,Mahshahr,Iran under the contract number 08-133/57665
文摘Desilication accompanied with minimum loss of crystallinity effect of a high alumina ZSM-5 zeolite on the isomerization reaction of ethylbenzene/xylene mixtures has been considered.Desilication was assessed through XRF,XRD,FTIR,TEM,nitrogen adsorption/desorption,NH_3-TPD,^(29)Si and^(27)Al MAS NMR analytical techniques.Desilication was accompanied with the creation of super acid sites.There exists a limit(Si/Al molar ratio of9.67)for keeping high crystallinity and obtaining improved catalytic performance.Desilication promotes ethylbenzene conversion by disproportionation and trans-alkylation reactions while the same reactions are limited for the xylene isomers.The p-xylene approach to equilibrium improves by more than 7% at 400℃ and a WHSV of 2 h^(-1)for the optimum sample with respect to the parent zeolite.At the same conditions,the optimum sample exhibits the maximum ethylbenzene conversion of 89%,i.e.more than 40%w.r.t.of the parent zeolite.However,the xylene yield decreases only 3%.
文摘MIL-125 is a metal-organic framework with great potential for the adsorption and separation of xylene isomers.However,MIL-125 is usually synthesized under anhydrous and anaerobic conditions.In this study,homogeneously shaped and highly crystalline MIL-125 was synthesized by introducing water-resistant titanium-containing oligomers into the synthesis process.With the assistance of the novel oligomers,MIL-125 can be synthesized in the presence of water,which meets batch-production requirements.The adsorption separation performance of the obtained highly crystalline MIL-125 was also significantly enhanced.The para-xylene/meta-xylene selectivity can reach 13.5 in mesitylene,which is higher than the selectivity values of most previously reported para-selective adsorbents.The MIL-125 xylene separation performance was verified using both batch adsorption and breakthrough experiments in the liquid phase.In addition,the influence of the solvent effect was evaluated through microcalorimetric experiments,liquid-phase adsorption experiments,and theoretical calculations.
文摘1. Introduction Zeolites are widely used in acid heterogeneous catalysis [1, 2]. Due to the unique physical and chemical properties ofzeolites, they are widely used in commercial catalytic processes, such as fluidized catalytic cracking, hydrocracking, methanol conversion to gasoline or olefins, ethylbenzene production, xylene isomerization, aromatics hydrogenation [3-9]. Acidity, high thermal stability, and shape selectivity determine the use of zeolites as catalysts in reaction processes through acid mechanisms [ 10].
