Electrocatalytic deep dehalogenation of florfenicol using Fe-doped CoP nanotubes array for blocking resistance gene expression and microbial inhibition during biochemical treatment

Abstract

Resistance gene expression and microbial inhibition by halogenated antibiotics is a major environmental concern. Although electrocatalytic dehalogenation can detoxify halogenated antibiotics, the effect of dehalogenation treatment on resistance gene expression and microbial inhibition is poorly understood. Herein, a novel electrocatalyst of Fe-doped CoP nanotubes array on nickel foam (Fe-CoP NTs/NiF) is prepared through a simple ultrasonication of Fe-doped CoP nanowires hydrothermally grown on NiF. The transformation from nanowires to nanotubes improves the crystallinity of CoP and fully exposes active sites, producing energetic atomic hydrogen for dehalogenation. Fe-CoP NTs/NiF exhibits a superior dehalogenation performance towards refractory florfenicol (FLO), achieving 100% removal within 20 min (‒1.2 V vs Ag/AgCl, C0 = 20 mg L‒1). The dechlorination ratio reaches nearly 100%, and the defluorination ratio achieves 36.8% within 50 min, showing the best electrocatalytic dehalogenation performance reported so far. Microbial community and correlation analysis show that Proteobacteria is the main potential host of FLO resistance gene. Electrocatalytic reductive dehalogenation pretreatment of FLO can reduce microbial inhibition, maintaining microbial richness and diversity in the subsequent biochemical treatment unit. The electrocatalytic reductive dehalogenation treatment can significantly reduce the relative abundance of FLO resistance gene, showing a reliable process for safe treatment of halogenated antibiotic containing wastewater.