含Re复合分子筛催化剂的制备及其在汽柴油加氢精制中的应用

发布时间：2018-02-03 02:30

  本文关键词： 含Re催化剂 复合分子筛 汽柴油 加氢精制 加氢脱芳　出处：《辽宁大学》2016年硕士论文　论文类型：学位论文

【摘要】：最近几年,随着全球变暖趋势的日益严重,越来越多的人们开始关注如何制造出一些对环境更为友好的燃料。汽柴油作为当今世界最重要的化石燃料之一,因此,如何更有效的降低其中含有的对环境有毒有害的物质的含量越发显得迫在眉睫。本文通过对一系列的含有新型载体的负载型催化剂的合成,首先,与汽柴油的模拟物四氢化萘在自制的仪器上进行了加氢精制脱芳反应,而后,再与汽柴油的模拟物四氢萘、噻吩、喹啉的混合物进行了深度脱芳脱氮脱硫,深度探究了汽柴油深度加氢精制的条件。主要做了以下四方面的工作：首先,通过改变催化剂的载体与(或)活性组分的配比与(或)组成,合成了新型的负载型的复合分子筛载体催化剂Mo-Re-Co/TiO2-USY-MCM-41,考察了汽柴油脱芳模拟物四氢萘在温度240-320℃、压力1.5-3.5 MPa、空速1-5 h-1、氢油比300-700的条件下,四氢萘的转换率最高可达到67.2%。其次,为了检验该催化剂对汽柴油加氢脱芳脱氮脱硫的实际效果,本文利用混合模拟物进行了深度加氢精制的反应。在最佳载体上负载不同的活性组分后,利用正交实验法找出最佳工艺条件后,在温度260℃、压力2.5 MPa、空速5 h-1、氢油比500的条件下进行加氢精制反应,噻吩的转换率可达到90.1%,喹啉的转换率为82.6%,四氢萘的转换率最高为62.7%。然后,将已得到的两种综合效果最好的催化剂进行复配结合,通过改变催化剂装填顺序的不同,进一步探究了原料油混合模拟物中三种物质的转换率。最后,对合成的复合载体及催化剂通过XRD、N2吸附-脱附进行了表征。其中,XRD表明复合载体中出现了新的物质组分Na0.3 [Al6(Si,Al)8O20(OH)10]·4H2O、 H12[(AlO2)12(SiO2)36]、Ti3O5和Al2SiO5,复合载体的N2吸附-脱附表现出了很好的介孔结构；同时,催化剂的活性金属组分也成功的负载在了所合成的复合载体上,达到了预期所要的结果。
[Abstract]:In recent years, with the increasing trend of global warming, more and more people begin to pay attention to how to make some more environmentally friendly fuels. Gasoline and diesel as one of the most important fossil fuels in the world today. Therefore, how to reduce the content of toxic and harmful substances is more and more urgent. In this paper, the synthesis of a series of supported catalysts containing new support, first of all. The hydrogenation of naphthalene from gasoline and diesel oil was carried out in a self-made instrument, and then the mixture of tetralin, thiophene and quinoline was used for deep denitrogenation and desulphurization with the mixture of naphthalene, thiophene and quinoline, which was the mimic of gasoline and diesel oil. The conditions of deep hydrogenation of gasoline and diesel oil were studied. The following four aspects were done: firstly, by changing the ratio and / or composition of catalyst carrier and / or active component. A novel supported composite molecular sieve support catalyst Mo-Re-Co/TiO2-USY-MCM-41 was synthesized. The dearomatization analogue tetralin was investigated under the conditions of temperature 240-320 鈩，

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