Effective degradation of phenol via catalytic wet peroxide oxidation over N, S, and Fe-tridoped activated carbon

Abstract

The N, S, and Fe-tridoped carbon catalysts (NSFe-Cs), Fe/ACNS1 and Fe/ACNS2, were synthesized by wet impregnation with different concentration of ammonium ferrous sulfate solution. The prepared catalysts have a similar textural structure. The N species, S species, Fe^II and Fe^III were simultaneously introduced onto the surface of catalysts. Comparison with the only Fe doped catalyst, NSFe-Cs showed greater stability and higher phenol removal in catalytic wet peroxide oxidation at different reaction condition. The main intermediates including p-hydroxybenzoic acid, formic acid, and maleic acid were determined in the treated wastewater. The high catalytic activity for NSFe-C was related to the ability of H₂O₂ decomposition. NSFe-Cs have more amount of Fe^II partially due to the formation of FeS₂, which promoted the decomposition of H₂O₂ on Fe/ACNS1 and Fe/ACNS2 surface. The generation of ·OH and ·HO₂/·O₂^- radicals in the bulk solution was crucial to phenol degradation, and the decomposition of H₂O₂ complied with the pseudo-first-order kinetics. The highly linear relationship between decomposition kinetic constant for H₂O₂ and the amount of surface groups suggested, including Fe^II species, pyridinic N/Fe-bonded N, pyrrolic N as well as graphitic N were responsible to the high activity of NSFe-Cs.

Keywords: Activated carbon; Ammonium ferrous sulfate; Heteroatom; Hydrogen peroxide; Phenol.