Experimental and theoretical assessment of bioinspired next-generation intercalated graphene oxide-based ceramic membranes for oil-in-water emulsion separation

Abstract

2D graphene oxide (GO) membranes are gaining prominence for water reclamation from oily wastewater. Unresolved challenges include low membrane permeance from tight sheets and fouling during separation. In this work, a bioinspired Arabic gum (AG) was used as an intercalated agent with the help of glutaraldehyde to improve the GO membranes’ permeation and fouling resistance. The 2D-laminated separating layer is crafted through a self-assembling innovative approach utilizing pressurized dead-end assembly. The Arabic gum intercalated graphene oxide-modified ceramic membrane (AGIGO-CM) appeared superhydrophilic and underwater (UW) superoleophobic with a UW oil contact angle (UWOCA) of 156.1 ± 1.2°. The membrane prepared with 1 mg of AGIGO (AGIGO-1-CM) offers a flux of 17 times higher than pristine graphene oxide (p-GO) while maintaining a separation efficiency of >99% during the separation of the oil-in-water emulsions. Molecular dynamics (MD) simulations showed AG intercalation expanding the interlayer distance by up to 20 Å, with AGIGO having a higher fractional free volume (FFV) of 0.986 compared to p-GO’s 0.599. AGIGO-CM displayed lower interfacial formation energy (EIFE) of −1865.2 kcal/mol versus −765.5 kcal/mol for p-GO, indicating easier separation. It is further supported by the substantial interfacial thickness of 148 Å for AGIGO-CM compared to 53.0 Å for the p-GO membranes. AGIGO-CM showed minimal fouling, retaining >99% separation efficiency for 6 h. Compared to p-GO-CM, AGIGO-CM flux decreased by only 17.84% versus 44.72%. AGIGO-CM exhibited stability even in acidic and basic environments, showcasing its potential for high performance.