High-efficiency removal of tetracycline from water by electrolysis-assisted NZVI: mechanism of electron transfer and redox of iron

Abstract

A low-cost, stable and non-precious metal catalyst for efficient degradation of tetracycline (TC), one of the most widely used antibiotics, has been developed. We report the facile fabrication of an electrolysis-assisted nano zerovalent iron system (E-NZVI) that achieved TC removal efficiency of 97.3% with the initial concentration of 30 mg L⁻¹ at an applied voltage of 4 V, which was 6.3 times higher than the NZVI system without an applied voltage. The improvement caused by electrolysis was mainly attributed to the stimulation of corrosion of NZVI, which accelerated the release of Fe²⁺. And Fe³⁺ in the E-NZVI system could receive electrons to reduce to Fe²⁺, which facilitated the conversion of ineffective ions to effective ions with reducing ability. Moreover, electrolysis assisted to expand the pH range of the E-NZVI system for TC removal. The uniformly dispersed NZVI in the electrolyte facilitated the collection and secondary contamination could be prevented with the easy recycling and regeneration of the spent catalyst. In addition, scavenger experiments revealed that the reducing ability of NZVI was accelerated in the presence of electrolysis, rather than oxidation. TEM-EDS mapping, XRD and XPS analyses indicated that electrolytic effects could also delay the passivation of NZVI after a long run. This is mainly due to the increased electromigration, implying that the corrosion products of iron (iron hydroxides and oxides) are not formed mainly near or on the surface of NZVI. The electrolysis-assisted NZVI shows excellent removal efficiency of TC and is a potential water treatment method for the degradation of antibiotic contaminants.