Adsorptive interaction of peroxymonosulfate with graphene and catalytic assessment via non-radical pathway for the removal of aqueous pharmaceuticals

Abstract

Graphene has been applied as a catalyst in peroxymonosulfate (PMS) activation for the removal of pharmaceuticals in water. Firstly, a kinetic adsorption study of PMS was developed, fitting the results to the Elovich’s equation. Moreover, the influence of the main variables in the adsorptive process such as pH, initial PMS concentration, and graphene dose were assessed. Secondly, the degradation of diclofenac as a target compound was studied comparing PMS-catalytic versus adsorption processes. PMS-catalytic process enhanced the removal of the micropollutant if compared to adsorption when using a low dose of graphene (less than 50 mg L−1) or after surface saturation. Studies using radical scavengers suggested the lack of radicals in the process, suggesting the non-radical activation of PMS. Thirdly, the adsorption versus PMS-catalytic processes were also compared for the oxidation of a mixture of three antibiotics (norfloxacin, tetracycline and sulfamethoxazole) with different chemical structure. PMS-catalytic activation was more effective for the removal of those compounds that presented less affinity towards adsorption onto the graphene surface. Finally, characterization of the fresh and PMS-treated material was performed. Graphene demonstrated to be stable after its use as catalysts in PMS activation, suffering only slight transformation of the surface oxidation groups.