Synthesis and Optimization of Superhydrophilic-Superoleophobic Chitosan–Silica/HNT Nanocomposite Coating for Oil–Water Separation Using Response Surface Methodology

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. (29)Si, (27)Al, and (13)H 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.