Facile Aerosol Synthesis and Characterization of Ternary Crumpled Graphene-TiO2-Magnetite Nanocomposites for Advanced Water Treatment

In this work, the synthesis and characterization of multifunctional crumpled graphene-based ternary nanocomposite photocatalysts for advanced water treatment applications is described. Currently, a major hurdle for the scale-up and optimization of aqueous, graphene-based photocatalysts is restacking of graphene nanosheets due to strong pi-pi interactions. To overcome this hurdle, a fast and facile aerosol technique to synthesize monomeric, aggregation-resistant, crumpled graphene-based photocatalysts was developed. The aerosol route utilizes water evaporation-induced confinement forces to effectively crumple graphene oxide and subsequently encapsulate commercially available TiO2 and magnetite nanoparticles. The as-synthesized crumpled graphene-TiO2-magnetite (GOTIM) ternary core-shell nanostructures are shown to possess superior aqueous-based photocatalytic properties (over a 20-fold enhancement in some cases) compared to TiO2 alone. Total GOTIM photocatalytic reactivity is confirmed to also include efficient photoreduction reaction pathways, in addition to expected oxidation routes typical of TiO2-based photocatalysts, significantly expanding photocatalytic application potential compared to TiO2 alone. Reaction kinetics and proposed mechanisms (both oxidative and reductive) are described for a model organic compound, here as methyl orange. Further, with the addition of hole scavengers such as EDTA, and/or lowering the O-2 concentration, we demonstrate enhancement of photocatalyzed reduction reactions, suggesting potential for directed, controlled reduction applications. In addition to robust aqueous stability, low-field magnetic susceptibility is demonstrated, allowing for low-energy, in situ material separations, which are critical for material recycling and reuse.