Chen Luohao, Liu Shuyan, Xu Zhijun, Yang Xiaoning
J Phys Chem Lett. 2019 Oct 3;10(19):5735-5741. doi: 10.1021/acs.jpclett.9b02074. Epub 2019 Sep 13.
Density functional theory simulations were carried out to study the binding interaction between hydrated Na/Cl and graphene oxide (GO) under electric fields. External electric fields can modify the binding interactions of the hydrated ions with GO. The field-dependent binding energy is mainly controlled by the orbital interaction driven by the field-dependent electron transfer, in which miscellaneous electron-transfer routes in the interfaces between hydrated ions and GO surface were disclosed. The electric field is able to influence the electron-transfer degree for each route, thereby creating various electron acceptor-donor coupling interactions. Furthermore, we preliminarily explored the effect of the electric field on the interlayer structure of bilayer GO with NaCl and water confined inside. Electric fields can enlarge the interlayer spacing through tuning of the hydrated ion-GO interactions. Our simulations present a new understanding of hydrated ion-GO interactions in the presence of an electric field, which is expected to be valuable in the electrical modulation of GO nanomaterials.
进行了密度泛函理论模拟，以研究电场作用下水合Na/Cl与氧化石墨烯（GO）之间的结合相互作用。外部电场可以改变水合离子与GO的结合相互作用。场依赖结合能主要由场依赖电子转移驱动的轨道相互作用控制，其中揭示了水合离子与GO表面界面处的多种电子转移途径。电场能够影响每条途径的电子转移程度，从而产生各种电子受体-供体耦合相互作用。此外，我们初步探索了电场对双层GO夹层结构的影响，其中NaCl和水被限制在夹层内。电场可以通过调节水合离子与GO的相互作用来扩大层间距。我们的模拟为电场存在下的水合离子与GO相互作用提供了新的理解，这有望在GO纳米材料的电调制中具有重要价值。
