Toward decentralized wastewater treatment: A flow-through module using microtubular gas diffusion electrodes for micropollutants removal.

Electro-Fenton (EF) represents an eco-friendly and cost-effective advanced oxidation process that can remove highly persistent and hazardous pharmaceuticals, e.g., contrast media agents, from water bodies. However, up to date, EF modules incorporate a planar carbonaceous gas diffusion electrode (GDE) cathode containing fluorinated compounds as polymeric binders. Here, we introduce a novel flow-through module that deploys freestanding carbon microtubes (CMT) as microtubular GDEs, omitting any risks of secondary pollution by highly-persistent fluorinated compounds (e.g., Nafion). The flow-through module was characterized for electrochemical hydrogen peroxide (H2O2) generation and micropollutant removal via EF. H2O2 electro-generation experiments illustrated high production rates (1.1 ± 0.1-2.7 ± 0.1 mg cm-2 h-1) at an applied cathodic potential of - 0.6 V vs. SHE, depending on the porosity of CMTs. Diatrizoate (DTZ), as the model pollutant, with a high initial concentration of 100 mg L-1 was successfully oxidized (95-100 %), reaching mineralization (TOC-total organic carbon removal) efficiencies up to 69 %. Additionally, Electro-adsorption experiments demonstrated the capability of positively charged CMTs to remove negatively charged DTZ with a capacity of 11 mg g-1 from a 10 mg L-1 DTZ solution. These results reveal the potential of the as-designed module to serve as an oxidation unit coupled with other separation techniques, e.g., electro-adsorption or membrane processes.