高硅铝比多级孔ZSM-11的合成及其在苯甲醇烷基化中的应用  

The synthesis of high Si/Al ratio hierarchical ZSM-11 and its catalytic properties on methylation of benzene

作　　者：董利荣 何暄[1] 杨帆[1] 朱学栋[1,2] Dong Lirong;He Xuan;Yang Fan;Zhu Xuedong(Engineering Research Center of Large Scale Reactor Engineering and Technology,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China;State Key Laboratory of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China)

机构地区：[1]华东理工大学化工学院大型工业反应器工程教育部工程研究中心,上海200237 [2]华东理工大学化学工程联合国家重点实验室,上海200237

出　　处：《石油化工》2018年第1期14-20,共7页Petrochemical Technology

摘　　要：结合溶剂挥发法和晶种法快速合成高硅铝比的多级孔ZSM-11分子筛,缩短了ZSM-11分子筛的合成周期,利用XRD、NH_3-TPD、N_2吸附和SEM等手段对合成的分子筛进行表征,考察了随着硅铝比的增加ZSM-11分子筛在苯甲醇烷基化反应中的催化性能。表征结果显示,随着硅铝比的增加,分子筛的比表面积和孔体积增加,酸量减少。实验结果表明,在410℃、0.18 MPa、WHSV=2 h^(-1)、n(苯)∶n(甲醇)=1的条件下,随硅铝比的增加,苯的转化率和二甲苯的选择性提高,乙苯的选择性降低,当硅铝比为180时,苯的转化率达到62.38%,二甲苯的选择性达到38.92%,乙苯的选择性降到0.21%;ZSM-11分子筛在150 h内仍保持较好的稳定性,具有较好的应用前景。The rapid synthesis of ZSM-11 zeolites with high Si/Al molar ratio by solvent evaporation and seeds-assisted methods is shortened the synthesis period of ZSM-11 zeolite.XRD,N2 adsorption,NH3-TPD and SEM were employed to characterize the structures and properties of the ZSM-11 samples.It was found that the samples had larger specific surface area and porous volume,lower acidity with the high molar ratio of Si/Al.The ZSM-11 zeolites were used as catalysts for benzene methylation under the conditions of 410℃,0.18 MPa and WHSV 2 h-1.It shows that with Si/Al increased from 30 to 180,the conversation of benzene and the selectivity to xylene increased,but the selectivity to ethylbenzene decreased.The catalyst with a Si/Al molar ratio of 180,its conversion of benzene reached 62.38%,the selectivity to xylene reached 38.92%,and the selectivity to ethylbenzene dropped to 0.21%.Meanwhile,the activity of hierarchical ZSM-11 is stable after 150 h on stream,with good prospects for the application.

关 键 词：高硅铝比 多级孔 ZSM-11 苯甲醇烷基化 

分 类 号：TQ426[化学工程]