Department of Chemistry , Louisiana State University , Baton Rouge , Louisiana 70803 , United States.
Université Grenoble Alpes, CNRS, DCM , 38000 Grenoble , France.
J Phys Chem B. 2019 Feb 21;123(7):1636-1649. doi: 10.1021/acs.jpcb.8b10987. Epub 2019 Feb 13.
The graphene oxide (GO)-water interface was simulated using Born-Oppenheimer molecular dynamics (BOMD) simulations with two different functionals, namely, revPBE-D3 and BLYP-D2, as well as a commonly used classical force field, namely, OPLS-AA. A number of different order parameters, including the orientation of the interfacial water molecules near the aromatic region of the GO surface as well as those near the oxygenated defects, were examined and compared. The BOMD interfacial waters are clearly much less structured as compared to the classical force field that shows a strongly ordered interface. Higher-level calculations, namely, symmetry adapted perturbation theory, were performed on representative clusters taken from the BOMD simulation. These calculations revealed not only that a number of conformations have similar interaction energies but also the importance of induction contribution to the interaction energies.
使用 Born-Oppenheimer 分子动力学 (BOMD) 模拟，结合两种不同的泛函，即 revPBE-D3 和 BLYP-D2，以及常用的经典力场 OPLS-AA，模拟氧化石墨烯 (GO)-水界面。研究并比较了许多不同的序参数，包括 GO 表面芳构区附近界面水分子的取向以及含氧缺陷附近的取向。与表现出强烈有序界面的经典力场相比，BOMD 界面水明显结构松散得多。对代表性团簇进行了更高层次的计算，即对称自适应微扰理论，这些计算不仅揭示了许多构象具有相似的相互作用能，还揭示了诱导贡献对相互作用能的重要性。
