Molecular Insight into the Adsorption Thermodynamics and Interfacial Behavior of GOs at the Liquid–Liquid Interface

The adsorption of two-dimensional (2-D) graphene oxide (GO) nanosheets at liquid-liquid interfaces has broad technological implications from functional material preparations to oil-water emulsification. Molecular-level understanding of the adsorption thermodynamics and the interfacial behavior is of great significance. Here, the adsorption free energy of GO nanosheets at the water-cyclohexane system was simulated, in which the effect of oxygen-containing groups and deprotonation has been investigated. It was observed that the neutral GO (GO-COOH) has obvious interfacial activity with a reduction of interfacial tension, while the deprotonated GO (GO-COO^-) shows a weak interface affinity. There exists an optimal oxidization degree that could cause the best interfacial stability, which is attributed to the balance of interfacial hydrophilic-hydrophobic interactions. The interaction arising from water is the main factor determining interfacial activity. The interfacial morphology and dynamics of GO nanosheets have also been simulated, in which an anisotropic 2-D translation and rotation along the interface were revealed. Our simulation results provide new insight into the adsorption mechanism and dynamics behavior of GO at the oil-water interface.