The
tardy Fe2+ regeneration and the limited pH range
confine the practical application of Fe-based homogenous Fenton-like
reaction performance. To surmount the abovementioned obstacles, we
applied molybdenum carbide (β-Mo2C) as the cocatalyst
to boost Fe3+ reduction in the activation of peroxydisulfate
(PDS) for the efficient degradation of dexamethasone (DXM). The proposed
Fe3+/PDS/β-Mo2C can remove more than 90%
DXM in the wide pH range (3.4 to 9.4). Electron spin resonance analysis
and probe and quenching tests comprehensively demonstrated that a
series of reactive species (•OH, SO4
•–, O2
•–, 1O2, and Fe(IV)) were formed during the synergistic
process, and SO4
•– was the leading
role. The circulation of Fe3+/Fe2+ was driven
by the exposed sites of Mo2+/Mo4+ on the β-Mo2C, which further promoted the PDS activation. The reaction
mechanism was clarified by various characterizations and density functional
theory calculation, which indicated that the adsorption between Fe3+ and β-Mo2C could form Mo–Fe bonds
and lengthen Fe–O and then improve the electron transport from
β-Mo2C to Fe3+ and boost Fe3+ reduction. The reactivity and stability of β-Mo2C was higher than those of popular Mo-based materials. This work
represents an attempt and possibility for Mo-based inorganic cocatalysis
of advanced oxidation processes.