石墨烯
曲面重建
空位缺陷
从头算
密度泛函理论
材料科学
范德瓦尔斯力
吸附
化学物理
共价键
表面能
分解
结晶学
计算化学
分子
曲面(拓扑)
物理化学
纳米技术
化学
几何学
复合材料
有机化学
数学
作者
Qian Wang,Rui Pang,Xingqiang Shi
标识
DOI:10.1021/acs.jpcc.5b06842
摘要
Inspired by experimental observations of Pt(111) surfaces reconstruction at the Pt/graphene (Gr) interfaces with ordered vacancy networks in the outermost Pt layer [e.g., Otero, G., et al. Phys. Rev. Lett. 2010, 105, 216102 ], the mechanism of the surface reconstruction is investigated by van der Waals corrected density functional theory in combination with particle-swarm optimization algorithm and ab initio atomistic thermodynamics. Our global structural search finds a more stable reconstructed structure than that which was reported before. With correction for vacancy formation energy, we demonstrate that the experimental observed surface reconstruction occurred at the earlier stages of graphene formation: (1) reconstruction occurred when C60 adsorption (before decomposition to form graphene) for C60 precursor or (2) reconstruction occurred when there were (partial) hydrogens remain in the hydrogenated precursors of C2H4 and planar C60H30. The reason is attributed to the fact that the energy gain, from the strengthened Pt–C partial sp3–like bonding for C of C60 or for C with partial H (than Pt–Gr bonding), compensates for the energy cost of formation surface vacancies and makes the reconstruction feasible, especially at elevated temperatures. In our predicted reconstructed structure Pt–C covalent bonds are formed that have a great impact on the adsorbed Gr electronic structures.
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