A series of ZSM-5@MCM-41 core-shell composite materials prepared via a multi-cycle-sol-gel coating strategy is investigated as the catalyst for benzene alkylation with ethylene,in which both ethylbenzene and para-diet...A series of ZSM-5@MCM-41 core-shell composite materials prepared via a multi-cycle-sol-gel coating strategy is investigated as the catalyst for benzene alkylation with ethylene,in which both ethylbenzene and para-diethylbenzene(p-DEB)are aimed as the target products.With multi-cycle-sol-gel coating,the external acid sites on the samples are gradually passivated by the inert MCM-41 shell.As a result,the shape selectivity to p-DEB is greatly enhanced.Nevertheless,the coating of mesoporous MCM-41 shell on ZSM-5 accelerates deactivation of the catalyst only due to the dilution effect of ZSM-5 content in the catalyst at the same space velocity,which is a reason that core-shell ZSM-5@MCM-41 will potentially be a practical catalyst in shape selective alkylation of benzene.In order to enhance the yield of p-DEB on ZSM-5@MCM-41,the reaction conditions at the fixed bed reactor including temperature,the molar rate of benzene to ethylene and GHSV,are also optimized.展开更多
Hierarchical ZSM-5 zeolite with radial mesopores is controllably synthesized using piperidine in a NaOH solution.The piperidine molecules enter the zeolite micropores and protect the zeolite framework from extensive d...Hierarchical ZSM-5 zeolite with radial mesopores is controllably synthesized using piperidine in a NaOH solution.The piperidine molecules enter the zeolite micropores and protect the zeolite framework from extensive desilication.The areas containing fewer aluminum atoms contain fewer piperidine protectant molecules and so they dissolve first.Small amounts of mesopores are then gradually generated in areas with more aluminum atoms and more piperidine protectant.In this manner,radial mesopores are formed in the ZSM-5 zeolite with a maximal preservation of the micropores and active sites.The optimal hierarchical ZSM-5 zeolite,prepared with a molar ratio of piperidine to zeolite of 0.03,had a mesopore surface area of 136 m·g and a solid yield of 80%.The incorporation of the radial mesopores results in micropores that are interconnected which shortened the average diffusion path length.Compared to the parent zeolite,the hierarchical ZSM-5 zeolite possesses more accessible acid sites and has a higher catalytic activity and a longer lifetime for the alkylation of benzene.展开更多
基金financial support by the National Natural Science Foundation of China(91534115)the National Key Research and Development Project(2016YFC1102300)。
文摘A series of ZSM-5@MCM-41 core-shell composite materials prepared via a multi-cycle-sol-gel coating strategy is investigated as the catalyst for benzene alkylation with ethylene,in which both ethylbenzene and para-diethylbenzene(p-DEB)are aimed as the target products.With multi-cycle-sol-gel coating,the external acid sites on the samples are gradually passivated by the inert MCM-41 shell.As a result,the shape selectivity to p-DEB is greatly enhanced.Nevertheless,the coating of mesoporous MCM-41 shell on ZSM-5 accelerates deactivation of the catalyst only due to the dilution effect of ZSM-5 content in the catalyst at the same space velocity,which is a reason that core-shell ZSM-5@MCM-41 will potentially be a practical catalyst in shape selective alkylation of benzene.In order to enhance the yield of p-DEB on ZSM-5@MCM-41,the reaction conditions at the fixed bed reactor including temperature,the molar rate of benzene to ethylene and GHSV,are also optimized.
基金the National Key Research and Development Program of China(Grant No.2017YFB0702800)China Postdoctoral Science Foundation(2016M600347).
文摘Hierarchical ZSM-5 zeolite with radial mesopores is controllably synthesized using piperidine in a NaOH solution.The piperidine molecules enter the zeolite micropores and protect the zeolite framework from extensive desilication.The areas containing fewer aluminum atoms contain fewer piperidine protectant molecules and so they dissolve first.Small amounts of mesopores are then gradually generated in areas with more aluminum atoms and more piperidine protectant.In this manner,radial mesopores are formed in the ZSM-5 zeolite with a maximal preservation of the micropores and active sites.The optimal hierarchical ZSM-5 zeolite,prepared with a molar ratio of piperidine to zeolite of 0.03,had a mesopore surface area of 136 m·g and a solid yield of 80%.The incorporation of the radial mesopores results in micropores that are interconnected which shortened the average diffusion path length.Compared to the parent zeolite,the hierarchical ZSM-5 zeolite possesses more accessible acid sites and has a higher catalytic activity and a longer lifetime for the alkylation of benzene.
