煤直接液化条件下菲催化加氢反应行为研究  

Catalytic Hydrogenation Reaction of Phenanthrene under Direct Coal Liquefaction Conditions

作　　者：王薇 舒歌平[1] 章序文[1] 王洪学[1] 高山松[1] 别士权 江洪波[2] WANG Wei;SHU Geping;ZHANG Xuwen;WANG Hongxue;GAO Shansong;BIE Shiquan;JIANG Hongbo(China Shenhua Coal to Liquid and Chemical Shanghai Research Institute,National Engineering Laboratory for Direct Coal Liquefaction,Shanghai 201108,China;Research Institute of Petroleum Processing,East China University of Science and Technology,Shanghai 200237,China)

机构地区：[1]中国神华煤制油化工有限公司上海研究院,煤炭直接液化国家重点实验室,上海201108 [2]华东理工大学石油加工研究所,上海200237

出　　处：《化学反应工程与工艺》2019年第2期106-112,共7页Chemical Reaction Engineering and Technology

基　　金：神华集团科技创新项目(SHJT-2017-17)。

摘　　要：为了开发将煤液化油中的重质芳烃组分经过预加氢处理后作为循环供氢溶剂工艺,以菲为模型化合物,在Ni-Mo/Al2O3催化剂上,利用恒温固定床反应器,进行了菲催化加氢反应行为研究。考察了不同体积空速(1.0~4.5 h^-1)、总压(14~20 MPa)、温度(300~400℃)对反应结果的影响,并结合Aspen平衡反应器模型对实验结果进行了分析。结果表明,实验条件下各反应均未达到热力学平衡。根据Langmuir-Hinshelwood-Hougen-Watson(LHHW)竞争吸附理论,计算了菲催化加氢的反应动力学,动力学结果表明,在煤直接液化条件下,Ni-Mo/Al2O3催化剂有利于菲的深度加氢,反应主要通过菲→二氢菲→八氢菲→全氢菲路径进行,可以通过适当增大空速和降低反应温度来控制菲的深度加氢,到达控制菲的加氢产物分布目的。To develop the process that the heavy aromatic component in the coal liquefied oil is taken as circulating of hydrogen-supply solvent by pre-hydrotreating,which has good hydrogen-supply performance,and the coal direct liquefaction reaction condition is mild with the circulating solvent.In the experiments,phenanthrene was used as a model compound,and the catalytic hydrogenation reactions of phenanthrene were studied on a Ni-Mo/Al2O3 catalyst using a constant-temperature fixed-bed reactor.The effects of different volume space velocity,pressure and temperature on the reaction results were investigated under the conditions of total pressure of 14-20 MPa and reaction temperature of 300-400℃,and the analysis with Aspen equilibrium reactor model showed that the hydrogenation reactions did not reach thermodynamic equilibrium under experimental conditions.According to Langmuir-Hinshelwood-Hougen-Watson(LHHW)competitive adsorption theory,the hydrogenation kinetics of phenanthrene reaction system were calculated.The kinetic data indicated that the Ni-Mo/Al2O3 catalyst is beneficial to the deep hydrogenation of phenanthrene under the direct coal liquefaction condition,and the reaction is mainly carried out through the path of phenanthrene→dihydrophenanthrene→octahydrophenanthrene→tetradecahydrophenanthrene.The depth of phenanthrene hydrogenation can be controlled by increasing the space velocity and lowering the reaction temperature appropriately to achieve the purpose of controlling the hydrogenation product distribution of phenanthrene.

关 键 词：煤直接液化 催化加氢 菲 动力学 

分 类 号：O643.1[理学—物理化学]