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Graphene oxide (GO) membranes with diverse lamellar distances can achieve sieving of molecules of different sizes in aqueous solutions. Without the extra assistance of cross-linking, the increase of lamellar distance supported by self-contained oxidized groups could diminish the internal π–π attraction force of GO membranes, resulting in the instability of GO membranes. However, the critical value of oxidized-group-supported lamellar distance of unstable GO membranes in aqueous solutions, which is crucial in applications for precise sieving of molecules, still remains unknown. In this study, the effect of oxidized-group-supported lamellar distance on the stability of graphene-based membranes in aqueous solutions is systematically investigated. By controlling the content of oxidized groups via changing reducing condition, different lamellar distances of graphene-based membranes are obtained. With changing the lamellar distance in aqueous solutions under different pH conditions, the graphene-based membranes show distinct stability. There exists a critical lamellar distance in the aqueous solution to ensure the stability of graphene-based membranes. If the lamellar distance is less than the critical value, the membranes remain physically stable for a long time, and still provide a favorable water permeation performance. The critical lamellar distances vary in aqueous solutions depending on pH values. The results provide a valuable guidance for the applications of graphene-based membranes in aqueous solutions.

Graphene oxide (GO) membranes become emerging efficient filters for molecular or ionic separation due to their well-defined two-dimensional nanochannels formed by closely spaced GO sheets and tunable physicochemical properties. The stability of GO membranes in aqueous solutions is a prerequisite for their applications. Here we show a novel and easy strategy for fabricating GO membranes with strong stability in aqueous solutions and controllable lamellar spacing by simply doping with partially reduced graphene oxide (prGO) sheets. With our prGO-doping strategy, the interlayer stabilizing force in GO membranes is enhanced due to the weakened repulsive hydration and enhanced π–π attraction between GO sheets; as a result, the fabricated GO membranes are featured with controllable lamellar spacing and extraordinary stability in water or even strong acid and base solutions as well as strong mechanical properties, which will expand the application scope of GO membranes and provide ever better performances in their applications with aqueous solution environments.