不同拓扑结构分子筛催化1-甲萘异构化-烷基转移耦合反应性能对比

Comparative study on the catalytic performance of zeolite catalysts with different topologies in 1-methylnaphthalene isomerization-transalkylation coupling reaction

  • 摘要: 以1-甲萘和均三甲苯为原料经固体酸催化的异构化-烷基转移耦合反应制备2-甲萘及二甲基萘。对MWW、BEA、FAU、MFI拓扑结构分子筛的催化性能进行对比研究,对反应机理进行探讨。采用XRD、BET、SEM、NH3-TPD、Py-FTIR及ICP等方法对催化剂结构物性进行了表征。与具有十元环特征孔道的MFI分子筛相比,具有十二元环特征孔道的MWW、BEA、FAU分子筛表现出更好的催化活性。BEA结构分子筛具有较高的二甲基萘选择性,而MWW结构分子筛具有较高的2-甲萘选择性并表现出优异的催化稳定性。在MWW结构分子筛中,HMCM-22的1-甲萘转化率达到70.27%,2-甲萘收率达到66.69%。而HMCM-56上则同时获得35.74%的2-甲萘收率和19.00%的二甲基萘收率。该研究为以中国丰富的碳十资源为原料制备高端聚酯单体2,6-二甲基萘开辟了颇具潜力的技术路线。

     

    Abstract: The isomerization-transalkylation coupling reaction between 1-methylnaphthalene and 1,3,5-trimethylbenzene was studied over zeolite catalysts to produce 2-methylnaphthalene and dimethylnaphthalene. The catalytic performance of zeolites with MWW, BEA, FAU and MFI topological structure was investigated and the reaction mechanism was discussed. The properties of zeolites were characterized by XRD, N2 adsorption-desorption, SEM, NH3-TPD, Py-FTIR and ICP. Compared with MFI zeolite with 10-membered ring channel, MWW, BEA and FAU zeolite with 12-membered ring channel showed better catalytic activity. BEA zeolite exhibited higher selectivity to dimethylnaphthalene, while MWW zeolites showed higher selectivity to 2-methylnaphthalene and the best catalytic stability. As a branch of MWW zeolites, HMCM-22 showed a 1-methylnaphthalene conversion of 70.27% and a 2-methylnaphthalene yield of 66.69%. It was worth noting that a relatively high yield of 2-methylnaphthalene (35.74%) and dimethylnaphthalene (19.00%) were obtained on HMCM-56 at the same time. This research has opened up a promising route using C10 aromatics as raw materials for the preparation of 2,6-dimethylnaphthalene, an important polyester monomer.

     

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