In this current study, facile, one-pot synthesis of functionalised nanocomposite coating with simultaneous hydrophilic and oleophobic properties was successfully achieved via the sol–gel technique. The synthesis of this nanocomposite coating aims to develop a highly efficient, simultaneously oleophobic-hydrophilic coating intended for polymer membranes to spontaneously separate oil-in-water emulsions, therefore, mitigating the fouling issue posed by an unmodified polymer membrane. The simultaneous hydrophilicity-oleophobicity of the nanocoating can be applied onto an existing membrane to improve their capability to spontaneously separate oil-in-water substances in the treatment of oily wastewater using little to no energy and being environmentally friendly. The synthesis of hybrid chitosan–silica (CTS-Si)/halloysite nanotube (HNT) nanocomposite coating using the sol–gel method was presented, and the resultant coating was characterised using FTIR, XPS, XRD, NMR, BET, Zeta Potential, and TGA. The wettability of the nanocomposite coating was evaluated in terms of water and oil contact angle, in which it was coated onto a polymer substrate. The coating was optimised in terms of oil and water contact angle using Response Surface Modification (RSM) with Central Composite Design (CCD) theory. The XPS results revealed the successful grafting of organosilanes groups of HNT onto the CTS-Si denoted by a wide band between 102.6–103.7 eV at Si^2p. FTIR spectrum presented significant peaks at 3621 cm⁻¹; 1013 cm⁻¹ was attributed to chitosan, and 787 cm⁻¹ signified the stretching of Si-O-Si on HNT. ²⁹Si, ²⁷Al, and ¹³H NMR spectroscopy confirmed the extensive modification of the particle’s shells with chitosan–silica hybrid covalently linked to the halloysite nanotube domains. The morphological analysis via FESEM resulted in the surface morphology that indicates improved wettability of the nanocomposite. The resultant colloids have a high colloid stability of 19.3 mV and electrophoretic mobility of 0.1904 µmcm/Vs. The coating recorded high hydrophilicity with amplified oleophobic properties depicted by a low water contact angle (WCA) of 11° and high oil contact angle (OCA) of 171.3°. The optimisation results via RSM suggested that the optimised sol pH and nanoparticle loadings were pH 7.0 and 1.05 wt%, respectively, yielding 95% desirability for high oil contact angle and low water contact angle.

Membrane filtration is an attractive process in water and wastewater treatment, but largely restricted by membrane fouling. In this study, the membrane fouling issue is addressed by developing polyethersulfone (PES)-based mixed matrix membranes (MMMs) with the incorporation of hydrophilic nanoparticles as an additive. Ultrafiltration MMMs were successfully fabricated by incorporating different loadings of halloysite nanotube-ferrihydrates (HNT-HFO) into a polyethersulfone (PES) matrix and their performance was evaluated for the separation of bovine serum albumin (BSA) solution and oil/water emulsion. The results show that wettability is endowed to the membrane by introducing the additive aided by the presence of abundant -OH groups from the HFO. The loading of additive also leads to more heterogeneous surface morphology and higher pure water fluxes (516.33–640.82 L/m²h) more than twice that of the pristine membrane as reference (34.69 L/m²h) without affecting the rejection. The MMMs also provide much enhanced antifouling properties. The filtration results indicate that the flux recovery ratio of the modified membrane reached 100% by washing with only distilled water and a total flux recovery ratio of >98% ± 0.0471 for HNT-HFO-loaded membranes in comparison with 59% ± 0.0169 for pristine PES membrane.