多环芳烃中苯的形成机理研究
Study on the formation mechanism of benzene in polycyclic aromatic hydrocarbons
作者：罗海银(长沙理工大学能源与动力工程学院)；曹小玲(长沙理工大学能源与动力工程学院)；田红(长沙理工大学能源与动力工程学院)；唐世斌(长沙理工大学能源与动力工程学院)；张航(长沙理工大学能源与动力工程学院)；熊家佳(长沙理工大学能源与动力工程学院)
Author：LUO Hai-Yin(School of Energy and Power Engineering, Changsha University of Science and Technology)；CAO Xiao-Ling(School of Energy and Power Engineering, Changsha University of Science and Technology)；TIAN Hong(School of Energy and Power Engineering, Changsha University of Science and Technology)；TANG Shi-Bin(School of Energy and Power Engineering, Changsha University of Science and Technology)；ZHANG Hang(School of Energy and Power Engineering, Changsha University of Science and Technology)；XIONG Jia-Jia(School of Energy and Power Engineering, Changsha University of Science and Technology)
收稿日期：2013-12-21 年卷（期）页码：2015,52(2):363-369
期刊名称：四川大学学报: 自然科学版
Journal Name：Journal of Sichuan University (Natural Science Edition)
关键字：多环芳烃; 苯; Gaussian09; 密度泛函理论
Key words：PAHs; Benzene; Gaussian09; Density functional theory
基金项目：国家自然科学基金(51276023); 国家自然科学基金国际(地区)合作与交流项目(51310105026)
中文摘要
为了研究多环芳烃中苯的形成过程, 设计了3条可能的反应路径, 采用Gaussian09中密度泛函的理论和UB3LYP/6 31＋＋G(d,p)基组进行计算, 以此为基础对苯的形成过程进行研究. 对反应物, 产物的几何构型进行优化, 通过TS方法寻找过渡态, 并用IRC路径分析验证了过渡态的可靠性. 计算了不同温度下的反应的热力学参数, 进行了热力学和动力学分析, 结果表明: 在不同温度下, 路径1,2,3的ΔH均小于零, 是放热反应, 随着反应温度增加, 焓变减少,反应放热增多, 且路径1,2的ΔG均小于零, 反应可自发进行, 随着温度增加, 反应物转化率变大, 而路径3的ΔG大于零, 反应基本不会进行. 比较3个反应路径的活化能, 所需活化能的大小顺序为1
英文摘要
In order to understand the forming process of benzene, three kinds of paths were designed by using density functional theory and UB3LYP/6 31 + + G (d, p) methods in Gaussian 09.The reactants and products were optimized by Gaussian 09, then the transition states can be found through the TS method, and the reliability of transition state also can be verified by IRC path analysis. Thermodynamic parameters in different temperatures were calculated to analysis the thermodynamic and kinetic properties. The calculation results show that path1, 2 and 3 are all exothermic reactions and the enthalpy changes are less than zero in different temperatures, The heat released along with temperature increasing and enthalpy changes decreasing, the gibbs free energy changes in path1 and 2 are less than zero, the reaction is spontaneous. The conversion of reactant raising with the increase of temperature, but gibbs free energy changes in path3 are more than zero, so the reaction does not exist. Comparing the activation energy in three paths, the order is 1
【关闭】
