磁性负载型超强酸催化的锡林浩特褐煤的加氢裂解

发布时间：2018-02-16 00:36

本文关键词： 三氟甲磺酸磁性负载型超强酸锡林浩特褐煤模型化合物催化加氢裂解　出处：《中国矿业大学》2016年硕士论文　论文类型：学位论文

【摘要】：煤是重要的重质碳资源,合理和有效地利用这一资源对于我国国民经济的可持续发展非常重要。了解煤的组成结构是有效利用煤的重要前提。煤的催化加氢裂解是研究煤的组成结构和以煤为原料获取高附加值产品的重要手段。本文以三氟甲磺酸(TFMS)和AlCl3为活性组分,二氧化硅包覆四氧化三铁为载体,制备磁性负载型超强酸催化剂,并用其催化煤相关模型化合物和煤的加氢裂解反应,并对反应产物进行分析。首先,制备磁性负载型超强酸催化剂。以FeSO4?7H2O和Fe2(SO4)3为原料,制备Fe3O4纳米粒子;再以正硅酸四乙酯(TEOS)为硅源,在碱性条件下缓慢水解生成二氧化硅包覆在Fe3O4纳米粒子周围,生成磁性载体;以甲苯为反应体系,加入TFMS、AlCl3和磁性载体,加热回流,制备磁性负载型超强酸催化剂。其次,以含有侧链的2-乙氧基萘(2-EN)和含有桥键的二苄醚(BE)做为模型化合物,以所制备的磁性负载型超强酸作为催化剂,初步探讨了2-EN和BE的催化加氢裂解反应的反应条件,同时讨论了二者的反应机理。结果显示,催化剂对BE的加氢裂解反应催化效果尤其明显,其反应可在温度低至413 K时进行;推测出2-EN和BE的催化加氢裂解反应机理为碳正离子机理;探索了催化加氢裂解反应的反应条件,确定了煤样的催化加氢裂解反应的反应条件,即加入1 g煤样,0.3 g催化剂,初始氢气压力为5 MPa。最后,使用催化剂催化了锡林浩特褐煤(XL)及其萃余煤(XER)和梁北烟煤(LB)及其萃余煤(LER)的加氢裂解反应,并对反应残渣进行了分级萃取。结果显示,在催化剂催化作用下,原煤和萃余煤加氢裂解反应收率均大于无催化剂存在下的反应收率;原煤和萃余煤的反应产物中酚类的种类和含量都明显高于无催化剂时酚类的种类和含量,说明催化剂对煤样加氢裂解反应中酚类的生成有很大的促进作用。
[Abstract]:Coal is an important heavy carbon resource, The rational and effective utilization of this resource is very important for the sustainable development of our national economy. Understanding the composition structure of coal is an important prerequisite for the effective utilization of coal. In this paper, TFMS and AlCl3 were used as active components. The magnetically supported superacid catalyst was prepared by using silica coated with iron trioxide as the carrier. The catalyst was used to catalyze the hydrocracking reaction of coal related model compounds and coal, and the products of the reaction were analyzed. Preparation of magnetic supported superacid catalyst. 7H2O and Fe2(SO4)3 were used as raw materials to prepare Fe3O4 nanoparticles, then tetraethyl tetraethyl orthosilicate (TEOS) was used as silicon source, which was hydrolyzed slowly under alkaline conditions to form silica coated around Fe3O4 nanoparticles to form magnetic carrier. Toluene was used as reaction system. The magnetic supported superacid catalyst was prepared by adding TFMSN AlCl3 and magnetic carrier to reflux. Secondly, 2-ethoxynaphthalene 2-en containing side chain and dibenzyl ether containing bridge bond were used as model compounds. Using the magnetic supported superacid as catalyst, the reaction conditions of 2-EN and be hydrocracking were preliminarily discussed, and the reaction mechanism of them was also discussed. The catalytic effect of the catalyst on the hydrocracking reaction of be is especially obvious, and the reaction can be carried out at a temperature of 413K, and the mechanism of 2-EN and be hydrocracking is deduced to be the mechanism of carbon positive ion. The reaction conditions of catalytic hydrocracking of coal samples were investigated. The reaction conditions of catalytic hydrocracking of coal samples were determined, that is, 1 g coal samples were added with 0.3 g catalyst, the initial hydrogen pressure was 5 MPA. The hydrogenation cracking reaction of Xilinhot lignite XERand Liangbei bituminous coal (LB) and its residual coal were catalyzed by catalyst, and the residue of the reaction was extracted by stages. The results showed that under the catalysis of catalyst, the hydrocracking reaction was carried out. The hydrocracking yield of raw coal and extracted residual coal was higher than that without catalyst, and the kinds and contents of phenols in the reaction products of raw coal and extracted residual coal were obviously higher than those without catalyst. The results show that the catalyst can promote the formation of phenols in the hydrocracking reaction of coal samples.
【学位授予单位】：中国矿业大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：TQ53;O643.3

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