Electrochemical degradation of antibiotics using flow-through graphene sponge electrodes

Abstract

Graphene sponge electrodes doped with atomic boron and nitrogen were employed for electrochemical degradation of antibiotics sulfamethoxazole, trimethoprim, ofloxacin, and erythromycin. The removal of antibiotics that displayed strong π-π interactions (i.e., ofloxacin) with reduced graphene oxide (RGO) coating was less limited by the mass transfer and removal efficiencies > 80% were observed for the investigated range of electrolyte flowrates. At the highest applied flowrate (700 LMH), increase in the anodic current significantly worsened the removal of trimethoprim and erythromycin due to the detrimental impact of the evolving gas bubbles. Increase in current at 700 LMH led to a stepwise increase in the removal efficiency of sulfamethoxazole due to its enhanced electrosorption. Electrochemical degradation was achieved via ozone, hydrogen peroxide and hydroxyl radical (•OH). Extraction of the employed graphene sponges confirmed the degradation of the strongly adsorbing antibiotics. Identified electrochemical transformation products of erythromycin confirmed the participation of •OH, through N-demethylation of the dimethylamine group. In real tap water, removal efficiencies were lower for all target antibiotics. Lower electric conductivity of tap water and thus increased thickness of the electric double layer likely limited their interaction with the graphene sponge surface, in addition to the presence of low amounts of organic matter