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偏三甲苯异构化制取均三甲苯研究

Research on the Production of1,3,5-trimethylbenzene by the Isomerization of1,2,4-trimethylbenzene

【作者】 王明

【导师】 王燕; 齐慧敏;

【作者基本信息】 天津大学 , 化学工程, 2014, 硕士

【摘要】 本文对以高纯偏三甲苯为原料异构化生产均三甲苯的工艺进行了研究,异构化反应以市售氢型丝光沸石(HM)为载体,以Ni/Mo和Ni/La为抑制积碳的金属组分,利用等体积浸渍法分别制备了Ni-Mo/HM和Ni-La/HM催化剂,并在加压固定床反应器上进行工艺研究。在Ni-Mo/HM催化剂上,分别考察了催化剂中Mo含量,反应温度,反应压力,质量空速,氢油比及催化剂寿命等因素对偏三甲苯异构化反应的影响。结果表明,催化剂中Mo含量为1.25%时,偏三甲苯异构化效果最好,偏三甲苯异构化反应最佳工艺条件为:反应温度260℃~270℃,反应压力1.2MPa~1.4MPa,质量空速0.9h-1~1.1h-1,氢油比5~6。在反应温度260℃,反应压力1.2MPa,质量空速1.0h-1,氢油比5的条件下,对Ni-Mo/HM催化剂进行连续200h运转,催化剂保持良好的活性和稳定性,没有失活迹象。采用XRD、Py-FTIR等分析手段对Ni-La/HM催化剂的结构和酸性质进行表征。并评价了La含量分别为0,0.63%,1.25%,1.88%和2.50%的C1,C2,C3,C4,C5五种Ni-La/HM催化剂在不同反应温度下偏三甲苯异构化的反应性能。结果表明,催化剂中La含量为1.25%,反应温度为240℃,反应压力1.2MPa,质量空速1.0h-1,氢油比5时,均三甲苯具有较高收率及选择性。负载抑制积碳的金属组分的氢型丝光沸石,不论是Ni-Mo/HM催化剂还是Ni-La/HM催化剂,均具有良好的催化活性和选择性,其稳定性也比纯氢型丝光沸石好,催化剂的使用寿命大大延长。

【Abstract】 The production of1,3,5-trimethylbenzene by the isomerization of1,2,4-trimethylbenzene was studied in this paper. In the experiment, the commercialhydrogen mordenite (HM) was used as the catalyst support. Ni/Mo and Ni/La wereused as metal components in retarding the coke formation. Catalysts Ni-Mo/HM andNi-La/HM were prepared by the incipient impregnation method. The synthesis werecarried out in the pressurized fixed-bed reactor.Firstly, the effects of Mo contents, reaction temperature, pressure, weight hourlyspace velocity (WHSV), hydrogen-oil ratio and the catalyst life on the isomerizationof1,2,4-trimethylbenzene over catalyst Ni-Mo/HM were studied. The results showedthat the Mo content is1.25%is the best condition for the isomerization of1,2,4-trimethylbenzene. And the optimal reaction conditions were obtained, whichwere the reaction temperature260℃~270℃, pressure1.2MPa~1.4MPa, WHSV0.9h-1~1.1h-1, and hydrogen-oil ratio5~6. Under the conditions of reactiontemperature260℃, reaction pressure1.2MPa, WHSV1.0h-1and hydrogen-oil ratio5, the Ni-Mo/HM catalyst had been reacted for200h, the catalyst kept good activityand stability and no catalyst deactivation sign had been found.Secondly, analytic technique, such as XRD and Py-FTIR, was used tocharacterize the structure and acidity of catalysts Ni-La/HM. Ctalytic performationof catalysts C1, C2, C3, C4and C5with La loading0,0.63%,1.25%,1.88%and2.50%respectively, were evaluated by the isomerization of1,2,4-trimethylbenzene atdifferent temperatures. The results showed that under the conditions of reactiontemperature240℃, reaction pressure1.2MPa, WHSV1.0h-1and hydrogen-oil ratio5, the Ni-La/HM catalyst had the best catalytic activity.The metal-loaded HM including catalyst Ni-Mo/HM and Ni-La/HM bothpossessed excellent catalytic activity and selectivity. The stability of them are betterthan the pure HM zeolite and the life of the catalysts was greately extended.

  • 【网络出版投稿人】 天津大学
  • 【网络出版年期】2016年 05期
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