Fe-g-C₃N₄/reduced graphene oxide lightless application for efficient peroxymonosulfate activation and pollutant...

To overcome the shortcomings of homogeneous Fe ion activating peroxymonosulfate (PMS), such as high pH-dependence, limited cycling of Fe(III)/Fe(II) and sludge production, graphite carbon nitride (g-C₃N₄) is chosen as a support for Fe ions, and reduced graphene oxide (rGO) is employed to facilitate the electron transfer process, thereby enhancing catalysis. Herein, a ternary catalyst, Fe-g-C₃N₄/rGO, is first applied under lightless condition for PMS activation, which exhibits ideal performance for contaminant mineralization. 82.5 % of the total organic carbon (TOC) in 100 mL of 5 mg/L bis-phenol A (BPA) was removed within 20 min by the optimal catalyst named 30%rFe_0.2CN, which shows a strong pH adaptability over the range of 3-11 compared with a common Fenton-like system. Moreover, the highly stable Fe-g-C₃N₄/rGO/PMS catalytic system resists complex water matrices, especially those with high turbidity. To unveil the mechanism of PMS activation and pollutant degradation, the physicochemical properties of the as-prepared catalysts are comprehensively characterized by multiple techniques. The Fe(III) contained in both the Fe-N group and α-Fe₂O₃ component of 30%rFe_0.2CN not only directly reacts with PMS to produce sulfate radicals (SO₄^-) and hydroxyl radicals (OH), but also combines with PMS to form the essential [Fe(III)OOSO₃]⁺ active complex, thereby generating superoxide radicals (O₂^-) and singlet oxygen (¹O₂). Among the various reactive oxidizing species, ¹O₂ plays an important role in pollutant removal, which is additionally generated by the CO moiety of the catalyst activating PMS as well as PMS self-oxidation, indicating the dominance of the non-radical pathway in the pollutant degradation process. Due to the advantages of high efficiency, wide pH adaptability and stability, the proposed lightless Fe-g-C₃N₄/rGO/PMS catalytic system represents a promising avenue for practical wastewater purification.