Rapid generation of high-valent cobalt-oxo species (Co(IV)O) for the removal of organic contaminants has been challenging because of the low conversion efficiency of Co(III)/Co(II) and the high activation energy barrier of the Co(II)-oxidant complex. Herein, we introduced nitrogen (N) vacancies into graphite carbon nitride imbedded with cobalt carbonate (CCH/CN−V n ) in a peroxymonosulfate (PMS)/visible light system to break the limitations of a conventional twoelectron transfer path. These N vacancies enhanced the electron distribution of the Co 3d orbital and lowered the energy barrier to cleave the O−O bond of PMS in the Co(II)-PMS complex, achieving the modulation of major active species from 1 O 2 to Co(IV)O. The developed synergistic system that exhibited adsorption and oxidation showed remarkable selectivity and contaminant removal performance in inorganic (Cl − , NO 3 − , HCO 3 − , and HPO 4 − ) organic (HA) and even practical aqueous matrices (tap water and secondary effluent). This study provides a novel mechanistic perspective to modulate the nonradical path for refractory contaminant treatment via defect engineering.
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