Superoleophilic, highly mechanically, and thermally stable electrospun membranes are promising for oil-water separation applications. This study aimed to fabricate a novel hydrophobic polyvinylidene fluoride/ZSM-5 (PVDF/ZSM-5) electrospun nanofiber composite membrane for gravity-driven oil-water separation and dye adsorption. Spinning parameters, including voltage, flow rate, tip-to-collector distance, solvent ratio, and polymer concentration, were systematically optimized, and composites with varying ZSM-5 loadings were fabricated. The membrane’s morphological characteristics were analyzed using field emission scanning electron microscopy (FESEM), while the influence of ZSM-5 on PVDF properties was investigated using Fourier transform infrared (FTIR) spectroscopy and Raman spectroscopy. The high thermal stability of the synthesized membrane was confirmed by thermogravimetric analysis (TGA), and an improvement in crystallinity was observed through X-ray diffraction (XRD) analysis. The incorporation of ZSM-5 enhanced the crystallinity and reduced the fiber diameter, thereby increasing the membrane’s surface area. Filler-matrix interactions were confirmed through FTIR, Raman, and TGA analyses. The addition of ZSM-5 improved the oil sorption capacity, achieving values in the range of 15–25 g/g, and increased the lab-scale oil flux to 341 L·m−2·h−1. Furthermore, the membrane exhibited effective adsorption of the toxic dye Congo red from water, following pseudo-first-order kinetics. Based on these findings, the PVDF/ZSM-5 composite membrane is a promising candidate for water purification applications, particularly in the removal of oil spills and organic solvents.
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