A series of Ferrierite(FER)zeolites were prepared via hydrothermal synthesis in the absence of organic templates with the aid of sodium-type FER zeolite(NaFER)or NaFER suspensions(NaFERsus)acquired by NaOH solution tr...A series of Ferrierite(FER)zeolites were prepared via hydrothermal synthesis in the absence of organic templates with the aid of sodium-type FER zeolite(NaFER)or NaFER suspensions(NaFERsus)acquired by NaOH solution treatment as seeds.The differences in the structures and acid sites of the obtained FER zeolite catalysts arising from the choice of seed were investigated,and the catalytic performances of the obtained FER zeolites were evaluated in the skeletal isomerization of n-butene.The results indicate that the samples synthesized using NaFERsus feature more Br?nsted acid sites(BAS)in the 10-membered-ring(10-MR)at the expense of strong acid and Lewis acid sites(LAS),compared with samples derived from NaFER.Therefore,the FER samples synthesized using NaFERsus outperformed the NaFER counterparts as the BAS in 10-MR and LAS were the main active sites,while BAS in 8-MR and LAS were responsible for side reactions,such as polymerization,cracking,and carbon deposition in n-butene isomerization.The optimized FER catalyst was continuously used for 720 h at 350℃ at 0.1 MPa under an n-butene space velocity of 2.0 h^(-1),during which the n-butene conversion remained at>40%,and the isobutylene yield was>37.5%.展开更多
The conversion of n-hexane and methanol into value-added aromatic compounds is a promising method for their industrially relevant utilization.In this study,intergrown ZSM-5/ZSM-11 crystals were synthesized and their r...The conversion of n-hexane and methanol into value-added aromatic compounds is a promising method for their industrially relevant utilization.In this study,intergrown ZSM-5/ZSM-11 crystals were synthesized and their resulting catalytic performance was investigated and compared to those of the isolated ZSM-5 and ZSM-1I zeolites.The physicochemical properties of ZSM-5/ZSM-l1 intergrown zeolite were analyzed using X-ray diffrac-tion,N2 isothermal adsorption-desorption,the tempera-ture-programmed desorption of ammonium,scanning clectron microscopy,Fourier transform infrared spectra of adsorbed pyridine,and nuclear magnetic resonance of 27AI,and compared with those of the ZSM-5 and ZSM-11 zeolites.The catalytic performances of the materials were evaluated during the co-feeding reaction of methanol and n-hexane under the fixed bed conditions of 400℃,0.5 MPa(N2),methanol:n-hexane=7:3(mass ratio),and weight hourly space velocity=1 h 1(methanol).Com-pared to the ZSM-5 and ZSM-11 zeolites,the ZSM-5/ZSM-11 zeolite exhibited the largest specific surface area,a unique crystal structure,moderate acidity,and suitable Brensted/Lewis acid ratio.The evaluation results showed that ZSM-5/ZSM-11 catalyst exhibited better catalytic reactivity than the ZSM-5 and ZSM-11 catalysts in terms of methanol conversion rate,n-hexane conversion rate,and aromatic selectivity.The outstanding catalytic property of the intergrown ZSM-5/ZSM-11 was attributed to the enhanced diffusion associated with its unique crystal.structure.The benefit of using zeolite intergrowth in the co-conversion of methanol and alkanes offers a novel route for future catalyst development.展开更多
基金the funding of the project by the CNPC Corporation (2018B-1907)。
文摘A series of Ferrierite(FER)zeolites were prepared via hydrothermal synthesis in the absence of organic templates with the aid of sodium-type FER zeolite(NaFER)or NaFER suspensions(NaFERsus)acquired by NaOH solution treatment as seeds.The differences in the structures and acid sites of the obtained FER zeolite catalysts arising from the choice of seed were investigated,and the catalytic performances of the obtained FER zeolites were evaluated in the skeletal isomerization of n-butene.The results indicate that the samples synthesized using NaFERsus feature more Br?nsted acid sites(BAS)in the 10-membered-ring(10-MR)at the expense of strong acid and Lewis acid sites(LAS),compared with samples derived from NaFER.Therefore,the FER samples synthesized using NaFERsus outperformed the NaFER counterparts as the BAS in 10-MR and LAS were the main active sites,while BAS in 8-MR and LAS were responsible for side reactions,such as polymerization,cracking,and carbon deposition in n-butene isomerization.The optimized FER catalyst was continuously used for 720 h at 350℃ at 0.1 MPa under an n-butene space velocity of 2.0 h^(-1),during which the n-butene conversion remained at>40%,and the isobutylene yield was>37.5%.
基金We gratefully acknowledge funding from the National Nature Science Foundation of China(Grant No.2177606)Technology administration of the Department of PetroChina Company Limited(2016-24308).
文摘The conversion of n-hexane and methanol into value-added aromatic compounds is a promising method for their industrially relevant utilization.In this study,intergrown ZSM-5/ZSM-11 crystals were synthesized and their resulting catalytic performance was investigated and compared to those of the isolated ZSM-5 and ZSM-1I zeolites.The physicochemical properties of ZSM-5/ZSM-l1 intergrown zeolite were analyzed using X-ray diffrac-tion,N2 isothermal adsorption-desorption,the tempera-ture-programmed desorption of ammonium,scanning clectron microscopy,Fourier transform infrared spectra of adsorbed pyridine,and nuclear magnetic resonance of 27AI,and compared with those of the ZSM-5 and ZSM-11 zeolites.The catalytic performances of the materials were evaluated during the co-feeding reaction of methanol and n-hexane under the fixed bed conditions of 400℃,0.5 MPa(N2),methanol:n-hexane=7:3(mass ratio),and weight hourly space velocity=1 h 1(methanol).Com-pared to the ZSM-5 and ZSM-11 zeolites,the ZSM-5/ZSM-11 zeolite exhibited the largest specific surface area,a unique crystal structure,moderate acidity,and suitable Brensted/Lewis acid ratio.The evaluation results showed that ZSM-5/ZSM-11 catalyst exhibited better catalytic reactivity than the ZSM-5 and ZSM-11 catalysts in terms of methanol conversion rate,n-hexane conversion rate,and aromatic selectivity.The outstanding catalytic property of the intergrown ZSM-5/ZSM-11 was attributed to the enhanced diffusion associated with its unique crystal.structure.The benefit of using zeolite intergrowth in the co-conversion of methanol and alkanes offers a novel route for future catalyst development.