Colloidal stability of modified graphene oxide (GO) is fundamental for its practical applications. Meanwhile, most of the investigations mainly focused on the nanosheets modified by a certain amount of modifiers and neglected the effects of the modification degree, which could vary the physical and chemical properties of modified GO and significantly affect its stability in solution. To the best of our knowledge, this study initially investigated the impact of modification degrees on the colloidal stability of graphene-based amphiphilic Janus nanosheets (JGO) via both experimental and theoretical approaches. The prepared JGO, asymmetrically grafted by dodecylamine, exhibited a direct relation between the modification degree and nanosheet thickness, refractive index, electrostatic properties, hydrophobicity, and the ultimate colloidal stability. In addition, the ionic strength imposed distinctive influences on the aggregation behavior of JGO. Based on the comparison between experimental results and theoretical calculation, it was revealed that the JGO should be modeled as twodimensional (2D) nanosheets in pure water and be treated as 3D spherical particles in electrolyte solutions for the prediction with the extended Derjaguin−Landau−Verwey−Overbeek theory.

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Various nanoparticles have been applied as chemical demulsifiers to separate the crude-oil-in-water emulsion in the petroleum industry, including graphene oxide (GO). In this study, the Janus amphiphilic graphene oxide (JGO) was prepared by asymmetrical chemical modification on one side of the GO surface with n-octylamine. The JGO structure was verified by Fourier-transform infrared spectra (FTIR), transmission electron microscopy (TEM), and contact angle measurements. Compared with GO, JGO showed a superior ability to break the heavy oil-in-water emulsion with a demulsification efficiency reaching up to 98.25% at the optimal concentration (40 mg/L). The effects of pH and temperature on the JGO’s demulsification efficiency were also investigated. Based on the results of interfacial dilatational rheology measurement and molecular dynamic simulation, it was speculated that the intensive interaction between JGO and asphaltenes should be responsible for the excellent demulsification performance of JGO. This work not only provided a potential high-performance demulsifier for the separation of crude-oil-in-water emulsion, but also proposed novel insights to the mechanism of GO-based demulsifiers.