Super-wetting MOFs@graphene hybrid has shown promising application for oil/water separation, due to high porosity, low density, and controllable wettability, however, achieving excellent stability and recyclability are found to be still challenging. In this study, sandwich-like UIO-66-F4@rGO hybrid was synthesized by immobilization of UIO-66-F4 nanoparticles on rGO matrix, which featured the unique micro/nano hierarchy with hydrophobic characteristics. In order to realize the oil/water separation, as-prepared sandwich-like UIO-66-F4@rGO hybrid was applied as a potential candidate for constructing robust super-hydrophobic/super-oleophilic interfaces by using filter paper (FP) and melamine sponge (MS) as substrates. Typically, the surface modification of substrates can be easily achieved by simple dip-coating method, and interfacial adhesion between substrates and UIO-66-F4@rGO was enhanced by cross-linking of hydroxyl-fluoropolysiloxane (FPSO). Consequently, the super-hydrophobic/oleophilic UIO-66-F4@rGO/FP exhibited high contact angle of 169.3 ± 0.6° and was capable of separating various water-in-oil emulsions effectively. The flux and separation efficiency were 990.45 ± 36.28 Lm−2 h−1 and 99.73 ± 0.19 % driven by gravity, respectively. The super-hydrophobic/super-oleophilic UIO-66-F4@rGO/MS possessed selective oil absorption with absorption capacity of 26∼61 g/g depending on the viscosity of oils and continuous cleaning of oil spill. Furthermore, the UIO-66-F4@rGO composite could tolerate high/low temperature, corrosive solutions, and physical damage, displaying robust and stable super-hydrophobic/super-oleophilic interfaces for treating oily wastewater in harsh environments.
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