Gao W, Zheng W T, Jiang Q
Key Laboratory of Automobile Materials, Ministry of Education, and Department of Materials Science and Engineering, Jilin University, Changchun 130022, People's Republic of China.
J Chem Phys. 2008 Oct 28;129(16):164705. doi: 10.1063/1.3001610.
The dehydrogenation of benzene on Pt(111) surface is studied by ab initio density functional theory. The minimum energy pathways for benzene dehydrogenation are found with the nudge elastic band method including several factors of the associated barriers, reactive energies, intermediates, and transient states. The results show that there are two possible parallel minimum energy pathways on the Pt(111) surface. Moreover, the tilting angle of the H atom in benzene can be taken as an index for the actual barrier of dehydrogenation. In addition, the properties of dehydrogenation radicals on the Pt(111) surface are explored through their adsorption energy, adsorption geometry, and electronic structure on the surface. The vibrational frequencies of the dehydrogenation radicals derived from the calculations are in agreement with literature data.
采用从头算密度泛函理论研究了苯在Pt(111)表面的脱氢反应。利用推挤弹性带方法找到了苯脱氢的最小能量路径，其中包括相关势垒、反应能、中间体和过渡态等几个因素。结果表明，在Pt(111)表面存在两条可能的平行最小能量路径。此外，苯中H原子的倾斜角可作为脱氢实际势垒的一个指标。另外，通过脱氢自由基在Pt(111)表面的吸附能、吸附几何结构和电子结构，对其性质进行了探索。计算得到的脱氢自由基的振动频率与文献数据一致。
