Persistent free radicals on N-doped hydrochar for degradation of endocrine disrupting compounds

Abstract

Metal-free carbocatalysts are raising increased interest in advanced oxidation processes (AOPs) for green degradation of aqueous organic pollutants. In the present study, a series of N-doped hydrochars (NHCs) was prepared from pinewood biomass and used in carbocatalysis toward catalytic peroxymonosulfate (PMS) activation to degrade refractory endocrine disrupting compounds. Nitrogen-doping was found to regulate the concentrations and types of persistent free radicals (PFRs) on hydrochar, promoting the electron transfer and oxidative degradation of the contaminants. Mechanistic studies revealed that graphitic N not only shows a strong electron transfer to facilitate PMS activation in a nonradical pathway, but also induces the formation of oxygen-centered PFRs from the structure defects for a radical oxidation pathway. More importantly, the PMS/NHC system demonstrates efficient degradation and satisfactory stability for real water treatment. This study has gained in-depth understanding on the roles of N-dopants in radical and nonradical pathways of biomass-based carbocatalysis, and will provide a promising and environmental-friendly route for efficient degradation of refractory endocrine disrupting compounds for green remediation.