A superhydrophilic and underwater superoleophobic PVDF membrane (PVDFAH) has been prepared by surface-coating of a hydrogel onto the membrane surface, and its superior performance for oil/water emulsion separation has been demonstrated. The coated hydrogel was constructed by an interfacial polymerization based on the thiol-epoxy reaction of pentaerythritol tetrakis (3-mercaptopropionate) (PETMP) with diethylene glycol diglycidyl ether (PEGDGE) and simultaneously tethered on an alkaline-treated commercial PVDF membrane surface via the thio-ene reaction. The PVDFAH membranes can be fabricated in a few minutes under mild conditions and show superhydrophilic and underwater superoleophobic properties for a series of organic solvents. Energy dispersive X-ray (EDX) analysis shows that the hydrogel coating was efficient throughout the pore lumen. The membrane shows superior oil/water emulsion separation performance, including high water permeation, quantitative oil rejection, and robust antifouling performance in a series oil/water emulsions, including that prepared from crude oil. In addition, a 24 h Soxhlet-extraction experiment with ethanol/water solution (50:50, v/v) was conducted to test the tethered hydrogel stability. We see that the membrane maintained the water contact angle below 5°, indicating the covalent tethering stability. This technique shows great promise for scalable fabrication of membrane materials for handling practical oil emulsion purification.

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Studies are conducted for the influence of the interface formation of graphene with various transition metals on its vibrational properties by using confocal micro-Raman spectroscopy. Micrometer-scale heterostructures consisting of patterned regions of the single layer and multilayer graphene (SLG and MLG, hereafter) covered with and without metals on the same graphene sheet were fabricated by thin-film deposition on the graphene surface through a shadow mask. Comparative analysis for these two different regions (SLG and MLG) fabricated within an identical graphene sheet enables us to investigate the interactions at and the doping effect from the metal/graphene interface as a function of the layers number of graphene without the influence of the unintentional doping. Confirmed dependences of the peaks shifts of the Raman bands (D, G, and 2D bands) on the graphene layers number and metal species (Co, Ni, and Au) reveal that the interfacial interactions are dramatically different between single layer and multilayer graphenes. In the metal/MLG heterostructures, the Raman band shifts are reasonably attributed to carrier doping from metals. It is found that the type of the doped carriers (electrons or holes) is different between Co/MLG and Au/MLG, irrespective of almost the same work functions of Co and Au. These analyses also provide the effective thickness of carrier doping (2-3 graphene layers) from the interfaces. In the metal/SLG heterostructures, significant differences from the metal/MLG heterostructures were observed for the Raman parameters of the G and 2D bands. It is suggested that there exist strong interactions at the metal/SLG interfaces different from those at the metal/MLG interfaces.