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Graphene oxide (GO) membranes have shown enormous promise in desalination and molecular/ionic sieving. However, the instability of GO membranes in aqueous solutions seriously hinders their practical applications. Herein, we report a novel and simple strategy to fabricate stable GO membranes in water-based environments through the insertion of various metal cations from metal foils (e.g., copper (Cu), iron (Fe), nickel (Ni), and zinc (Zn) foils) and natural deposition. Based on the cation-π, coordination, and electrostatic interaction between metal cations and GO nanosheets, the aqueous stability and mechanical strength of the membranes are significantly improved. The permeation rates for acetone, toluene, and p-xylene molecules across the GO membrane cross-linked by copper ions with a deposition time of 24 h are 0.966, 0.074, and 0.100 mol m-2 h-1, respectively. Moreover, this membrane displays excellent separation performance, and the separation factor of K+/Mg2+ is up to 68.8 in mono-/multivalent metal cation sieving, which indicate the effective molecular/ionic sieving performance. Meanwhile, the ionic sieving of the GO membrane cross-linked by copper ions has excellent repeatability and long-term stability. The versatility of this natural deposition strategy to fabricate GO membranes cross-linked by metal cations is investigated by using Fe foil, Zn foil, and Ni foil as well as other porous substrates such as polyvinylidene fluoride (PVDF), polyethersulfone (PES), and nylon membranes and filter paper. This fabrication strategy also enables low-cost preparation of large-area GO membranes. Therefore, GO membranes cross-linked by metal cations and prepared by this simple metal cation incorporation strategy have large potential application for molecular/ionic sieving in various solution systems.

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.