分子筛催化甲基萘烷基化反应的研究
张凤
学位类型硕士
导师高志贤 ; 吾满江·艾力
2011-05-30
学位授予单位中国科学院研究生院
学位授予地点北京
学位专业有机化学
关键词Β分子筛 改性 甲基萘 烷基化
摘要

本文以2-甲基萘(2-MN)为原料,经烷基化合成混合二烷基萘,以提高二烷基萘的总选择性为目标,具体研究内容和结果如下: (一)以甲醇作烷基化试剂,探讨了无溶剂的体系和以TMB作溶剂的反应体系。考察了HZSM-5和Mg、Co改性β分子筛催化剂和反应温度条件的影响,初步获得了甲醇烷基化的反应规律。 (二)以乙醇作烷基化试剂,研究Hβ及Zn、Mg、Co改性的β分子筛作催化剂,反应体系(2-MN+乙醇+TMB)在一系列温度下的反应,深入探讨和比较了各种催化剂的催化性能。重点研究了Co/Hβ分子筛催化剂上2-MN的烷基化反应,考察了Co含量、反应温度的影响。通过与Hβ、Zn/Hβ、Mg/Hβ分子筛对比,可以发现反应温度为400℃~450℃,1%Co/Hβ分子筛上2-MN的转化率较高,目的产物二烷基萘的总选择性较高,副产物萘和多烷基萘较少。 (三)通过对比实验,即(2-MN+TMB)在催化剂上的转化,研究了烷基化反应过程,产物二烷基萘的来源,以及甲醇或乙醇作为烷基化试剂参与反应的程度。 (四)通过甲醇、乙醇各自单独转化的实验结果可知,甲醇生成的甲烷较多,致使催化剂失活且速率较快,乙醇主要生成乙烯,有利于烷基化反应。 (五)结合甲醇、乙醇作烷基化试剂和对比实验结果,证实烷基化过程中发生包括异构化、歧化、烷基化等反应;产物二烷基萘大多来源于2-MN的歧化和均三甲苯的转移烷基化,甲醇或乙醇作为烷基化试剂部分参与了2-MN的烷基化反应,而相当一部分则生成了低碳烃。

其他摘要

The process for preparing dialkylnaphthalenes by alkylation of 2-methylnaphthalene (2-MN) over zeolite catalyst was studied aiming at obtaining high selectivity to dialkylnaphthalenes. The main results of this thesis are summarized as following: (1) The alkylation of 2-MN with methanol or with (methanol + TMB) was discussed. The performance of HZSM-5 and Mg or Co modified Hβ zeolite catalysts and the influence of reaction temperature were studied. (2) The reaction system of (2-MN+ethanol+1,3,5-TMB) was investigated over Hβ and Zn, Mg, Co modified Hβ zeolite catalysts at different reaction temperature. The effects of different catalysts were compared and discussed. The alkylation of 2-MN was mainly studied over Co modified Hβ zeolite catalysts, and the influences of reaction temperature and Co loading on the catalytic performance were investigated. Compared with Hβ, Zn/Hβ and Mg/Hβzeolites, 1%Co/Hβ showed both better conversion and selectivity to dialkylnaphthalenes at 400℃-450℃ reaction temperature range. (3) The process of alkylation, the source of dialkylnaphthalenes and the contribution of alkylation with methanol or ethanol as alkylation regent were investigated according to the transformation results of reactant mixture of 2-MN and TMB over zeolite catalyst. (4) The results of reaction of methanol or ethanol showed that methanol generated much methane and ethanol produced a lot of ethylene. (5) Upon further additional tests, it was found that the process consisted several reactions such as isomerization, disproportionation and alkylation. It was demonstrated that the formation of dialkylnaphthalenes mainly resulted from both the disproportionation of 2-MN and the transfer alkylation with TMB, and the contribution of alkylation by methanol or ethanol was small as compared with that transformed to lower hydrocarbons.

文献类型学位论文
条目标识符http://ir.xjipc.cas.cn/handle/365002/4435
专题新疆维吾尔自治区精细化工工程技术研究中心
作者单位中国科学院新疆理化技术研究所
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张凤. 分子筛催化甲基萘烷基化反应的研究[D]. 北京. 中国科学院研究生院,2011.
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