Self-templated method to synthesize hierarchical pore ZSM-5 and its application in MTA reaction
TONG Xin1, WEI Zhen-hao1, ZHU Xue-dong1,2
1. Engineering Research Center of Large Scale Reactor Engineering and Technology of the Ministry of Education, East China University of Science and Technology, Shanghai 200237, China; 2. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
Abstract: Mesoporous silica sphere prepared by the modified Stober method is used as silicon source and hard template to synthesize hierarchical pore ZSM-5 molecular sieve with Si/Al ratio of 30.The obtained samples are characterized by XRD,FESEM,N2 adsorption-desorption and NH3-TPD.The effects of temperature,time and method of crystallization on the morphology and structural performance of molecular sieve are investigated.The catalytic performance of samples is evaluated through applying to methanol to aromatics (MTA) reaction.The results show that the ZSM-5 molecular sieve with high crystallinity can be made through using mesoporous silica sphere as silicon source and hard template and performing crystallization at 110℃ for 72 h.This molecular sieve has rich mesopores and macropores with a specific surface area of 529 m2·g-1,and exhibits better catalytic stability in MTA reaction.
佟鑫, 魏振浩, 朱学栋. 自模板法制多级孔ZSM-5及其在MTA反应中的应用[J]. 现代化工, 2018, 38(5): 150-154.
TONG Xin, WEI Zhen-hao, ZHU Xue-dong. Self-templated method to synthesize hierarchical pore ZSM-5 and its application in MTA reaction. Modern Chemical Industry, 2018, 38(5): 150-154.
[1] 李静,刘粟侥,张怀科,等.特殊形貌类雪花状ZSM-5分子筛的合成、表征及甲醇烯烃催化性能[J].催化学报,2016,2:308-315. [2] 孙翔宇.ZSM-5分子筛的合成、后处理及其在苯与甲醇烷基化中的应用[D].上海:华东理工大学,2013. [3] 张荣荣,王正宝.后处理改性对HZSM-5沸石丁烯裂解性能的影响[J].化工学报,2015,66(8):3098-3015. [4] Schwieger W,Machoke A G,Reiprich B,et al.Hierarchy concepts:Classification and preparation strategies for zeolite containing materials with hierarchical porosity[J].Chem Soc Rev,2016,45:3353-3376. [5] Cui Tian-lu,Li Xin-hao,Lv Li-bing,et al.Nanoscale Kirkendall growth of silicalite-1 zeolite mesocrystals with controlled mesoporosity and size[J].Chemical Communications,2015,(51):12563-12566. [6] Albert G Machoke,Ana M Beltránr,et al.Micro/Macroporous system:MFI-Type zeolite crystals with embedded macropores[J].Adv Mater,2015,27:1066-1070. [7] Stober W,Fink A.Controlled growth of monodisperse silica spheres in the micron size range[J].J Colloid Interf Sci,1968,26:62-69. [8] Aguayo A T,Mier D,Gayubo A G,et al.Kinetics of methanol transformation into hydrocarbons on a HZSM-5 Zeolite catalyst at high temperature (400~550℃)[J].Industrial and Engineering Chemistry Research,2010,49(24):12371-12378. [9] 王杰.胶体晶体的制备及研究[D].济南:山东师范大学,2009. [10] 徐如人,庞文琴,等.分子筛与多孔材料化学[M].北京:科学出版社,2004. [11] 陆璐,张会贞,朱学栋.多级孔ZSM-5分子筛的合成及催化苯甲醇烷基化反应的研究[J].石油学报(石油加工),2012,S1:111-115. [12] Tao Y,Kanoh H,Abrams L,et al.Mesopore-modified zeolites:Preparation,characterization,and applications[J].Chemical Reviews,2006,106(3):896-910. [13] Kim J C,Ryoo R,Opanasenko M V,et al.Mesoporous MFI zeolite nanosponge as a high-performance catalyst in the pechmann condensation reaction[J].ACS Catalysis,2015,5(4):2596-2604. [14] Zhou J,Liu,Z LI Liyuan,et al.Hierarchical mesoporous ZSM-5 zeolite with increased external sites and high catalytic performance in o-xylene isomerization[J].Chinese Journal of Catalysis,2013,34:1429-1433. [15] 马利勇,林晓云,李宏峰,等.基于ZSM-5的多级孔分子筛合成研究进展[J].化工生产与技术,2014,21(5):27-32,8.