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.

Molecular transport through nanopores has recently received considerable attention as a result of advances in nanofabrication and nanomaterial synthesis technologies. Surprisingly, water transport investigations through carbon nanochannels resulted in two contradicting observations: extremely fast transport or rejection of water molecules. In this paper, we elucidate the mechanism of impeded water vapor transport through the interstitial space of aligned multiwalled carbon nanotubes (aligned-MWCNTs)--capillary condensation, agglomeration, reverse capillary flow, and removal by superhydrophobicity at the tip of the nanotubes. The origin of separation comes from the water's phase change from gas to liquid, followed by reverse capillary flow. First, the saturation water vapor pressure is decreased in a confined space, which is favorable for the phase change of incoming water vapor into liquid drops. Once continuous water meniscus is formed between the nanotubes by the adsoprtion and agglomeration of water molecules, a high reverse Laplace pressure is induced in the mushroom-shaped liquid meniscus at the entry region of the aligned-MWCNTs. The reverse Laplace pressure can be significantly enhanced by decreasing the pore size. Finally, the droplets pushed backward by the reverse Laplace pressure can be removed by superhydrophobicity at the tip of the aligned-MWCNTs. The analytical analysis was also supported by experiments carried out using 4 mm-long aligned-MWCNTs with different intertube distances. The water rejection rate and the separation factor increased as the intertube distance decreased, resulting in 90% and 10, respectively, at an intertube distance of 4 nm. This mechanism and nanotube membrane may be useful for energy-efficient water vapor separation and dehumidification.

Soft conductive materials should enable large deformation while keeping high electrical conductivity and elasticity. The graphene oxide (GO)-based sponge is a potential candidate to endow large deformation. However, it typically exhibits low conductivity and elasticity. Here, the highly conductive and elastic sponge composed of GO, flower-shaped silver nanoparticles (AgNFs), and polyimide (GO-AgNF-PI sponge) are demonstrated. The average pore size and porosity are 114 µm and 94.7%, respectively. Ag NFs have thin petals (8-20 nm) protruding out of the surface of a spherical bud (300-350 nm) significantly enhancing the specific surface area (2.83 m g ). The electrical conductivity (0.306 S m at 0% strain) of the GO-AgNF-PI sponge is increased by more than an order of magnitude with the addition of Ag NFs. A nearly perfect elasticity is obtained over a wide compressive strain range (0-90%). The strain-dependent, nonlinear variation of Young's modulus of the sponge provides a unique opportunity as a variable stiffness stress sensor that operates over a wide stress range (0-10 kPa) with a high maximum sensitivity (0.572 kPa ). It allows grasping of a soft rose and a hard bottle, with the minimal object deformation, when attached on the finger of a robot gripper.

Here we present a new strategy of selectively rejecting water vapor while allowing fast transport of dry gases using temperature-controlled aligned-multiwalled carbon nanotubes (aligned-MWNTs). The mechanism is based on the water vapor condensation at the entry region of nanotubes followed by removing aggregated water droplets at the tip of the superhydrophobic aligned-MWNTs. The first condensation step could be dramatically enhanced by decreasing the nanotube temperature. The permeate-side relative humidity was as low as ∼17% and the helium-water vapor separation factor was as high as 4.62 when a helium-water vapor mixture with a relative humidity of 100% was supplied to the aligned-MWNTs. The flow through the interstitial space of the aligned-MWNTs allowed the permeability of single dry gases an order of magnitude higher than the Knudsen prediction regardless of membrane temperature. The water vapor separation performance of hydrophobic polytetrafluoroethylene membranes could also be significantly enhanced at low temperatures. This work combines the membrane-based separation technology with temperature control to enhance water vapor separation performance.

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