Ma Yuan, Gao Lei, Yan Yu, Su Yanjing, Qiao Lijie
Corrosion and Protection Center, Key Laboratory for Environmental Fracture (MOE), University of Science and Technology Beijing Beijing 100083 China
RSC Adv. 2018 Mar 27;8(21):11807-11812. doi: 10.1039/c8ra00735g. eCollection 2018 Mar 21.
To achieve the chemical modification of graphene efficiently is desirable and essential to promote the technological applications of graphene. In this study, the density functional theory (DFT) calculations have been carried out to investigate the hydrogenation and fluorination activities of graphene on Ni(111), Re(0001) and Pt(111). The calculation results indicate that the chemical activity of graphene is related to both the characteristics of the graphene-substrate interfacial interaction and the local atomic stacking, namely the chemical activity of graphene is position-dependent. The strong covalently interacting substrates Ni(111) and Re(0001) will remarkably enhance the chemical activity of graphene, while the modulation effects from the weak van der Waals interacting substrate Pt(111) is trivial. Electronic structure studies reveal that the intensive graphene-substrate interfacial interaction can gain in chemical energy to offset the strain energy caused by the C atom sp-sp transition and stabilize the absorbing state.
高效实现石墨烯的化学修饰对于推动石墨烯的技术应用而言是可取且至关重要的。在本研究中，已进行密度泛函理论（DFT）计算，以研究石墨烯在Ni(111)、Re(0001)和Pt(111)上的氢化和氟化活性。计算结果表明，石墨烯的化学活性与石墨烯 - 衬底界面相互作用的特性以及局部原子堆积均有关，即石墨烯的化学活性是位置依赖的。强共价相互作用的衬底Ni(111)和Re(0001)将显著增强石墨烯的化学活性，而弱范德华相互作用的衬底Pt(111)的调制效应微不足道。电子结构研究表明，强烈的石墨烯 - 衬底界面相互作用可获得化学能以抵消由C原子sp - sp跃迁引起的应变能，并稳定吸附态。
