甲醇耦合抽余油芳构化反应催化剂制备及其催化性能研究  

PREPARATION AND PERFORMANCE OF CATALYST FOR AROMATIZATION OF METHANOL COUPLING WITH RAFFINATE

作　　者：魏书梅 徐亚荣 李琪蓉 朱学栋[1] Wei Shumei;Xu Yarong;Li Qirong;Zhu Xuedong(Engineering Research Center of Large Scale Reactor Engineering and Technology,East China University of Science and Technology,Shanghai 200237;PetroChina Urumqi Petrochemical Company Research Institute)

机构地区：[1]华东理工大学工业大型反应器工程教育部工程研究中心,上海200237 [2]中国石油乌鲁木齐石化公司研究院

出　　处：《石油炼制与化工》2021年第6期11-17,共7页Petroleum Processing and Petrochemicals

基　　金：国家自然科学基金资助项目(27176076)。

摘　　要：采用简单、快速、易工业化的一步法水热合成制备了ZSM-5 ZSM-11共晶分子筛,采用X射线衍射、N 2吸附-脱附、NH 3程序升温脱附、吡啶吸附红外光谱、扫描电镜和透射电镜等分析手段对ZSM-5 ZSM-11共晶分子筛进行了表征,并将成型催化剂应用于催化甲醇耦合抽余油芳构化反应体系中。结果表明:通过一系列表征手段证实了合成的分子筛为ZSM-5 ZSM-11共晶分子筛,具有多级孔结构,其比表面积为358 m 2 g,孔体积0.35 cm 3 g;具有B酸和L酸,B酸L酸酸量比为2.07,晶体是由棒状的六方柱体插接而成的规则、棱角清晰的球体构成。在反应温度为380℃、反应压力为0.5 MPa、甲醇抽余油质量比为1∶1、质量空速为1 h-1的条件下,ZSM-5 ZSM-11共晶分子筛成型催化剂催化甲醇耦合抽余油芳构化反应时,C 5+收率大于81%,芳烃收率最高为38%。ZSM-5 ZSM-11共晶分子筛催化剂催化甲醇耦合抽余油芳构化反应具有良好的工业应用前景。Co-crystallized ZSM-5 ZSM-11 zeolite was prepared by one-step hydrothermal method,which was simple,rapid and easy to be industrialized.The samples were characterized by XRD,N 2 adsorption-desorption,Py-IR,SEM and TEM techniques.The results showed that the synthesized sample was ZSM-5 ZSM-11 co-crystallization zeolite with hierarchical pore structure,specific surface area of 358 m 2 g,pore volume of 0.35 cm 3 g,and B L acid amount ratio of 2.07.And the crystal was composed of regular,sharp-edged spheres with rod-shaped hexagonal cylinders.The formulated catalyst,by mixing the ZSM-5 ZSM-11 zeolites with alumina,was used in the aromatization reaction of methanol coupling with raffinate.Under the conditions of a reaction temperature of 380℃,a reaction pressure of 0.5 MPa,a mass ratio of methanol to raffinate of 1∶1 and a mass space velocity of 1 h-1,the yield of C 5+was over 81%with the yield of aromatics up to 38%.Therefore,the ZSM-5 ZSM-11 co-crystallization zeolite has a good industrial application prospect in the catalytic aromatization of methanol coupling with raffinate.

关 键 词：ZSM-5/ZSM-11共晶分子筛 多级孔 甲醇 抽余油 芳构化 

分 类 号：TQ241[化学工程—有机化工] TQ426