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  本文關(guān)鍵詞： 三氟甲磺酸 磁性負載型超強酸 錫林浩特褐煤 模型化合物 催化加氫裂解　出處：《中國礦業(yè)大學》2016年碩士論文　論文類型：學位論文

【摘要】：煤是重要的重質(zhì)碳資源,合理和有效地利用這一資源對于我國國民經(jīng)濟的可持續(xù)發(fā)展非常重要。了解煤的組成結(jié)構(gòu)是有效利用煤的重要前提。煤的催化加氫裂解是研究煤的組成結(jié)構(gòu)和以煤為原料獲取高附加值產(chǎn)品的重要手段。本文以三氟甲磺酸(TFMS)和AlCl3為活性組分,二氧化硅包覆四氧化三鐵為載體,制備磁性負載型超強酸催化劑,并用其催化煤相關(guān)模型化合物和煤的加氫裂解反應(yīng),并對反應(yīng)產(chǎn)物進行分析。首先,制備磁性負載型超強酸催化劑。以FeSO4?7H2O和Fe2(SO4)3為原料,制備Fe3O4納米粒子;再以正硅酸四乙酯(TEOS)為硅源,在堿性條件下緩慢水解生成二氧化硅包覆在Fe3O4納米粒子周圍,生成磁性載體;以甲苯為反應(yīng)體系,加入TFMS、AlCl3和磁性載體,加熱回流,制備磁性負載型超強酸催化劑。其次,以含有側(cè)鏈的2-乙氧基萘(2-EN)和含有橋鍵的二芐醚(BE)做為模型化合物,以所制備的磁性負載型超強酸作為催化劑,初步探討了2-EN和BE的催化加氫裂解反應(yīng)的反應(yīng)條件,同時討論了二者的反應(yīng)機理。結(jié)果顯示,催化劑對BE的加氫裂解反應(yīng)催化效果尤其明顯,其反應(yīng)可在溫度低至413 K時進行;推測出2-EN和BE的催化加氫裂解反應(yīng)機理為碳正離子機理;探索了催化加氫裂解反應(yīng)的反應(yīng)條件,確定了煤樣的催化加氫裂解反應(yīng)的反應(yīng)條件,即加入1 g煤樣,0.3 g催化劑,初始氫氣壓力為5 MPa。最后,使用催化劑催化了錫林浩特褐煤(XL)及其萃余煤(XER)和梁北煙煤(LB)及其萃余煤(LER)的加氫裂解反應(yīng),并對反應(yīng)殘渣進行了分級萃取。結(jié)果顯示,在催化劑催化作用下,原煤和萃余煤加氫裂解反應(yīng)收率均大于無催化劑存在下的反應(yīng)收率;原煤和萃余煤的反應(yīng)產(chǎn)物中酚類的種類和含量都明顯高于無催化劑時酚類的種類和含量,說明催化劑對煤樣加氫裂解反應(yīng)中酚類的生成有很大的促進作用。
[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.
【學位授予單位】：中國礦業(yè)大學
【學位級別】：碩士
【學位授予年份】：2016
【分類號】：TQ53;O643.3

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本文編號：1514250