The presence of pharmaceuticals and personal care products (PPCPs) in aquatic systems is a serious threat to human and ecological health. The photocatalytic degradation of PPCPs via titanium oxide (TiO2) is a well-researched potential solution, but its efficacy is limited by a variety of environmental conditions, such as the presence of natural organic macromolecules (NOM). In this study, we investigate the synthesis and performance of a novel photoreactive composite: a three-dimensional (3D) core (TiO2)-shell (crumpled graphene oxide) composite (TiGC) used as a powerful tool for PPCP removal and degradation in complex aqueous environments. TiGC exhibited a high adsorption capacity (maximum capacity 11.2 mg/g, 100 times larger than bare TiO2) and a 30% enhancement of photodegradation (compared to bare TiO2) in experiments with a persistent PPCP model, carbamazepine (CBZ). Furthermore, the TiGC performance was tested under various conditions of NOM concentration, light intensity, CBZ initial concentration, and multiple cycles of CBZ addition, in order to illustrate that TiGC performance is stable over a range of field conditions (including NOM). The enhanced and stable performance of TiCG to adsorb and degrade CBZ in water extends from its core-shell composite nanostructure: the crumpled graphene oxide shell provides an adsorptive surface that favors CBZ sorption over NOM, and optical and electronic interactions between TiO2 and graphene oxide result in higher hydroxyl radical (•OH) yields than bare TiO2.
Keywords: PPCPs removal; carbamazepine photodegradation; core-shell structured catalyst; environmental photocatalysis; spray drying technology; titanium dioxide graphene composite.