芘加氢的分子模拟研究

Molecular simulation on hydrogenation of pyrene

石油资源短缺和原油重质化、劣质化的趋势,以及不断上涨的对清洁油品的需求,使得通过加氢充分利用石油中多环芳组分成为近期石油炼制工业研究的热点问题。本文采用量子力学方法对模型化合物芘的加氢位置及反应历程进行了考察,结果表明,芘倾向于在端环边位先加氢,有三条主要的加氢路径。在反应初期,中间环边位碳原子的加氢稍占优势,但随着反应的深入进行继续加氢困难。模拟计算结果与不同温度下芘在NiMo催化剂上加氢得到的反应产物分布试验数据吻合较好。

Along with the shortage of oil,its quality was getting poorer.However,the demand for clean oil products was rising sharply.Making full use of polycyclic aromatic components in oil through hydrogenation had become a hot issue in petroleum refining industry.In this paper, quantum mechanical methods were used to locate the sites of C atoms where hydrogenation happened and investigate reaction mechanism of pyrene hydrogenation.It was found that the hydrogenation of pyrene tended to occur on side rings prior to center rings,and there were three reaction paths mainly.However,at the beginning of reactions,H free radicals preferred to react with C atoms on sides of center rings.As the reactions continued,further hydrogenations got to be difficult.The experimental data of the product distribution obtained from the reactions of pyrene hydrogenation carrying on NiMo catalyst in different temperatures was in good agreement with the simulation results.