以溴甲烷为甲基化试剂制备二甲苯的催化研究
首发时间:2011-01-08
摘要:采用商购ZSM-5分子筛及其改性样品作为催化剂,探讨溴甲烷作为甲基化试剂甲基化甲苯制备二甲苯的可行性。系统考察了分子筛硅铝比、改性剂以及改性剂负载量对ZSM-5分子筛催化活性与选择性的影响,还探究了反应温度、甲苯质量空速以及原料配比等因素对甲苯转化率及二甲苯收率的影响规律。研究结果表明:在甲苯甲基化制备二甲苯反应中,溴甲烷作为甲基化试剂较甲醇更具有优势;当分子筛硅铝比为100,反应温度为400℃,甲苯质量空速为0.46h-1,甲苯与溴甲烷的摩尔比为1:1时,二甲苯的收率达到最高(29.3%);HZSM-5分子筛经Mg、B、P改性后,对二甲苯在二甲苯中的选择性均高于热力学平衡值24%。
关键词: 工业催化 溴甲烷 甲苯 ZSM-5分子筛 甲基化 二甲苯
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Study on catalytic synthesis of xylene using methyl bromide as methylation agent
Abstract:In order to achieve an effective use of natural gas resources to get higher value-added aromatics products, we examined the catalytic synthesis of xylene by methylation of toluene using methyl bromide as methylation agent in the presence of ZSM-5 zeolite on a fixed-bed reactor. The effects of SiO2/Al2O3 ratio, reaction temperature, weight hourly space velocity of toluene and toluene/CH3Br molar ratio on toluene conversion and xylene yield were systematically investigated. The yield of xylene is up to 29.3% under the optimal reaction condition (SiO2/Al2O3 ratio, reaction temperature, weight hourly space velocity and toluene/CH3Br molar ratio are 100, 400oC, 0.46h-1 and 1, respectively). CH3Br as methylation agent is more effective than methanol for the methylation of toluene into xylene. Furthermore, p-xylene selectivity in xylene is higher than the thermodynamic equilibrium value after the HZSM-5 molecular sieve catalysts are modified by Mg, B or P compound.
Keywords: industral catalysis CH3Br toluene HZSM-5 methylation xylene
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No.4403006426723129****
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