Enhanced peroxymonosulfate activation on dual active sites of N vacancy modified g-C3N4 under visible-light assistance and its selective removal of organic pollutants

Abstract

Constructing highly efficient metal-free material towards peroxymonosulfate (PMS) activation under photocatalytic assistance is a promising strategy for water decontamination. Herein, N vacancy modified g-C3N4 nanotube (VCN) was prepared to build a novel photo-assisted PMS activation system (PPAS), in which the unique electronic structure created by N vacancy could favor the PMS activation on VCN under visible-light irradiation. The role of N vacancy in PPAS was firstly studied through tuning its content in VCN. The results showed that the N vacancy greatly improved PMS activation on VCN PPAS towards organic pollutants removal. The VCN PPAS with moderate N vacancy modification performed best, whose kinetic constant for Rhodamine B degradation was 9.6 and 2.6 times higher than that of VCN/PMS system and pristine g-C3N4 PPAS, respectively. Moreover, the VCN PPAS performed well in wide pH range (3−12) and real water background. Selective removal of different organic pollutants was found on VCN PPAS, owing to the different interaction between pollutant and the catalyst surface with surface-bound radicals. The O2− and OH were major oxidants for pollutant removal in VCN PPAS, which were produced on dual active sites of VCN via two pathways: The N vacancy enhanced PMS adsorption and trapped photogenerated electrons for PMS reduction into OH, while the electron-deficient C atoms created by N loss promoted the PMS oxidation into O2−.