Magnetic recoverable MnFe₂O₄ and MnFe₂O₄-graphene hybrid as heterogeneous catalysts of peroxymonosulfate activation for efficient degradation of aqueous organic pollutants.

Abstract

Magnetic iron based materials are generally effective for many catalytic reactions and can be magnetically recovered after application, showing advantages than other metal oxides. In the present work, magnetic MnFe2O4 nanoparticle and MnFe2O4-reduced graphene oxide (rGO) hybrid were prepared and used as catalysts to activate peroxymonosulfate (PMS) to oxidatively degrade various organic pollutants in water. From a process of chemical deposition and reduction, MnFe2O4-rGO hybrids were produced with nanosized MnFe2O4 particles (ca. 13.2 nm). It was found that MnFe2O4 or MnFe2O4-rGO presented high activity in activating PMS to produce sulfate radicals for degradation of organic dyes (Methyl violet, Methyl orange, Methylene blue, Orange II and Rhodamine B) and could be separated with a magnet without any loss. The reaction kinetics, effect of different ion species CL(-),HCO3(-),CH3COO(-)and NO3(-) and Cl(-) strength, reaction temperature (25-65°C), catalytic stability, as well as degradation mechanism were comprehensively studied. The lower activation energy on MnFe2O4-rGO (25.7 kJ/mol) justify the higher chemical performance than that of MnFe2O4 (31.7 kJ/mol), suggesting that graphene plays a significant role in the enhanced degradation of dyes. More importantly, the as-prepared MnFe2O4 and MnFe2O4-rGO hybrid exhibited stable performance to remove the organic pollutants in wastewater with easy recycling and good stability by successive degradation experiments.