空壳型ZSM-5分子筛用于苯-乙醇烷基化制乙苯的研究  

Alkylation of benzene with ethanol to ethylbenzene over bowl-like hollow ZSM-5 zeolite catalysts

作　　者：张雅飞 朱鹏 张雄福[1] 张媛 夏飞 张伟[2] ZHANG Ya-fei;ZHU Peng;ZHANG Xiong-fu;ZHANG Yuan;XIA Fei;ZHANG Wei(State Key Laboratory of Fine Chemicals,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,China;Xi'an Clean Energy(Chemical)Research Institute of ACS Dalian Institute of Chemical Physics,Shaanxi Yanchang Petroleum(Group)Co.,Ltd.,Xi'an 710075,China)

机构地区：[1]大连理工大学化工学院,精细化工国家重点实验室,辽宁大连116024 [2]陕西延长石油(集团)有限责任公司大连化物所西安洁净能源(化工)研究院,陕西西安710075

出　　处：《现代化工》2023年第1期185-191,197,共8页Modern Chemical Industry

基　　金：陕西延长石油(集团)有限责任公司大连化物所西安洁净能源(化工)研究院资助项目(JJ0521SKF0001)。

摘　　要：选用空壳型ZSM-5分子筛为母体催化剂,利用固定床反应器考察了煤基乙醇与苯烷基化制备乙苯反应条件对催化性能的影响,并在优化条件下评价空壳型HZSM-5母体催化剂的反应稳定性;研究了水热处理与P或Zn单组分对母体ZSM-5联合改性所得催化剂的烷基化催化性能。结果表明,空壳型HZSM-5母体催化剂用于苯与乙醇烷基化反应,连续反应100 h性能基本没有变化,苯转化率保持在13.4%左右、乙基选择性为97.8%,而二甲苯相对质量分数保持在3400μg/g。经过单组分改性与水热处理联合改性的空壳型HZSM-5分子筛,可以进一步提高乙基选择性和降低二甲苯杂质质量分数,在苯/乙醇摩尔比为6、反应温度为340℃和空速为6 h-1的优化条件下,苯转化率大于10%,乙基选择性大于99%,二甲苯相对质量分数低于700μg/g,具有很好的应用开发潜力。Based on the alkylation of benzene with ethanol to ethylbenzene,bowl-like hollow ZSM-5 is selected as parent catalyst to evaluate the reaction in a fixed-bed reactor.The reaction conditions are optimized for the alkylation over HZSM-5 parent catalyst.Then,the catalytic performance of the catalyst obtained by modifying the parent ZSM-5 with both hydrothermal treatment and P or Zn component is evaluated in the alkylation.The results show that the catalytic performance of HZSM-5 parent catalyst remains unchanged after having experienced continuous reaction for 100 h.The conversion of benzene is maintained at about 13.4%,the selectivity of ethyl is 97.8%,and the mass fraction of xylene is kept at 3400μg·g-1.The modified catalyst by both hydrothermal treatment and single component can further increase the selectivity of ethyl and reduce the mass fraction of xylene,over which the conversion of benzene exceeds 10%,the selectivity of ethyl exceeds 99%,and the relative mass fraction of xylene is less than 700μg·g-1when the molar ratio of benzene to ethanol is 6,the reaction temperature is 340℃and the space velocity is 6 h-1.Therefore,the modified hollow ZSM-5 catalyst has excellent application and development potential.

关 键 词：分子筛 ZSM-5 烷基化反应 乙苯 催化剂改性 

分 类 号：O643[理学—物理化学]