化学
钴
吸附
电子转移
水溶液
光化学
无机化学
碳纤维
键裂
催化作用
有机化学
材料科学
复合数
复合材料
作者
Jingjing Jiang,Ziqing Zhao,Jiaying Gao,Tianren Li,Mingyu Li,Dandan Zhou,Shuangshi Dong
标识
DOI:10.1021/acs.est.2c01913
摘要
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-Vn) in a peroxymonosulfate (PMS)/visible light system to break the limitations of a conventional two-electron 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 1O2 to Co(IV)═O. The developed synergistic system that exhibited adsorption and oxidation showed remarkable selectivity and contaminant removal performance in inorganic (Cl-, NO3-, HCO3-, and HPO4-) 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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