Janus Graphene Oxide Sponges for High-Purity Fast Separation of Both Water-in-Oil and Oil-in-Water Emulsions

Membrane separation of oil and water with high purity and high permeability is of great interest in environmental and industrial processes. However, membranes with fixed wettability can separate only one type of surfactant-stabilized emulsion (water-in-oil or oil-in-water). Here, we report on Janus graphene oxide (J-GO) sponges for high purity and high permeability separation of both water-in-oil and oil-in-water emulsions. Millimeter-scale reduced GO sponges with a controlled pore size (11.2 or 94.1 μm) are synthesized by freeze drying, and the wettability is further controlled by fluorine (hydrophobic/oleophilic in air) or oxygen (hydrophilic/oleophilic in air) functionalization. J-GO sponges are prepared by the fluorine functionalization on one side and oxygen functionalization on the other side. Interestingly, the oil wettability of oxygen-functionalized surface turns into an oleophobic surface when immersed in water, which is explained by Young's theory. This effect is further used in the separation of both water-in-oil and oil-in-water emulsions by changing the flow direction. The purity of the separated oil and water is very high (≥99.2%), and the permeability is more than an order of magnitude greater than those of the other Janus membranes reported. J-GO sponges can be reused with an excellent repeatability, demonstrating feasibility in practical applications.