Oxygen vacancy-induced nonradical degradation of nitroso-containing organics in Fe3O4@N[sbnd]C electro-Fenton reaction at a wide pH range

Abstract

In this work, Fe3O4-anchored nitrogen-doped carbon catalyst (Fe3O4@NC) with abundant oxygen vacancies (Vo) and mesoporous structure was successfully synthesized for electro-Fenton (EF) catalytic process. The catalyst demonstrated impressive degradation efficiency towards nitroso-containing organics due to the superior electronic transfer of NC skeleton and Vo, making it easier for the electron-deficient –NO2 groups to adsorb on the catalyst surface and oxidize rapidly. Typically, the degradation efficiency of p-nitrophenol (PNP) reached 95.8 % in natural pH. Notably, the catalyst exhibited excellent performance over a wide pH range (3 ∼ 11), and has strong anti-interference performance against anions and natural organic matter in water matrix. Mechanism analysis indicated that Vo could promote the formation of highly active electron-rich Fe(II) species, and promote the activation of H2O2 and O2 as additional active sites, thus, a large amount of ·OH and O2·- would be produced and then quickly converted into 1O2. As a result, 1O2 is the main reactive species for PNP degradation in Fe3O4@NC electro-Fenton reaction. The results will provide insights into the design of high-performance catalysts for the selective oxidation of organic pollutants in wastewater.