Scalable fabrication of robust superhydrophobic membranes by one-step spray-coating for gravitational water-in-oil emulsion separation

Hydrophobic anti-wetting membranes have many applications, such as oily wastewater treatment via oil/water separation, desalination via membrane distillation, and carbon capture via gas-liquid membrane contactors. Herein, we used a simple and scalable method to fabricate robust superhydrophobic polyvinylidene fluoride (PVDF) based membranes by one-step spray-coating of fluorinated SiO 2 nanoparticles. The prepared PVDF membrane was systematically characterized by Fourier transform infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy and contact angle measurements. The modified PVDF membrane had excellent superhydrophobicity with an extremely high water contact angle up to 171.8 ± 1.1° and a low sliding angle of 1.69 ± 0.13°, due to the fluorinated close-packed hydrophobic SiO 2 nanoparticles on the surface. The modified PVDF membrane maintained its relatively stable superhydrophobicity under various harsh conditions, i.e., exposure in hot water, NaOH and HCl, ultrasonication and high-speed flushing, indicating the superior robustness and stability. The prepared membrane also exhibited consistent separation efficiencies up to 99.88 ± 0.03% in water-in-oil emulsions, and superior recyclability and durability over 40 cycles. In addition, spray-coating showed its great promise in engineering various superhydrophobic surfaces on different substrates and excellent scalability in fabricating large-size membranes. This study demonstrates a facilely scalable spray-coating method for engineering robust superhydrophobic surfaces and membranes that can be potentially used for various gas, vapor and water/oil separations.