Hierarchical ZSM-5 zeolites with intercrystalline mesopores are crucial for improving the mass transport and accessibility of active sites.Traditional synthesis methods often require organic structure-directing agents...Hierarchical ZSM-5 zeolites with intercrystalline mesopores are crucial for improving the mass transport and accessibility of active sites.Traditional synthesis methods often require organic structure-directing agents with complicated design and/or environmentally harmful additives while involving tedious synthetic procedures.To streamline the method for constructing hierarchical ZSM-5 zeolites,we herein propose a seed-induced approach free of any additives to efficiently synthesize oriented nanorod-assembled hierarchical ZSM-5 zeolites(NA-ZSM-5)with abundant intercrystalline mesopores.By systematically examining the parameters of the seed on the resultant ZSM-5,we found that a seed with high crystallinity is a prerequisite for constructing the oriented aggregation of nanorods while the length of the nanorods can be finely controlled from∼180 nm to∼600 nm via adjusting the seed dosage.Importantly,the seed functions as a dynamic template on which aluminosilicate precursors gradually deposit and further evolve to c-axis oriented nanorods.The resulting NA-ZSM-5 zeolite demonstrates a relatively better catalytic lifetime of 200 h,with benzene conversion constantly higher than 53.3%and ethyl selectivity remaining above 92.4%in the benzene alkylation with ethanol.Additionally,this synthetic procedure can be successfully scaled up in 1 L and 3 L autoclaves with product yields of above 94%.This work demonstrates an efficient and scalable approach to producing hierarchical ZSM-5 zeolites with abundant intercrystalline mesopores for value-added conversion of the benzene series.展开更多
基金the Joint Project of Dalian University of Technology–Dalian Institute of Chemical Physics(Grant No.HX20230236)Natural Science Foundation of Liaoning Province(No.2025-BS-0030)the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(No.E301190101)for supporting this work.
文摘Hierarchical ZSM-5 zeolites with intercrystalline mesopores are crucial for improving the mass transport and accessibility of active sites.Traditional synthesis methods often require organic structure-directing agents with complicated design and/or environmentally harmful additives while involving tedious synthetic procedures.To streamline the method for constructing hierarchical ZSM-5 zeolites,we herein propose a seed-induced approach free of any additives to efficiently synthesize oriented nanorod-assembled hierarchical ZSM-5 zeolites(NA-ZSM-5)with abundant intercrystalline mesopores.By systematically examining the parameters of the seed on the resultant ZSM-5,we found that a seed with high crystallinity is a prerequisite for constructing the oriented aggregation of nanorods while the length of the nanorods can be finely controlled from∼180 nm to∼600 nm via adjusting the seed dosage.Importantly,the seed functions as a dynamic template on which aluminosilicate precursors gradually deposit and further evolve to c-axis oriented nanorods.The resulting NA-ZSM-5 zeolite demonstrates a relatively better catalytic lifetime of 200 h,with benzene conversion constantly higher than 53.3%and ethyl selectivity remaining above 92.4%in the benzene alkylation with ethanol.Additionally,this synthetic procedure can be successfully scaled up in 1 L and 3 L autoclaves with product yields of above 94%.This work demonstrates an efficient and scalable approach to producing hierarchical ZSM-5 zeolites with abundant intercrystalline mesopores for value-added conversion of the benzene series.
