Iron- and cobalt-based
heterogeneous catalysts are widely applied
for activating peroxymonosulfate (PMS) to degrade organic pollutants.
However, few studies have unveiled the clear synergistic mechanism
of iron and cobalt in ZSM-5. In this paper, the synergistic mechanism
of enhanced PMS activation was revealed by constructing iron and cobalt
bimetal modified ZSM-5 zeolite catalysts (FeCo-ZSM-5). The tetracycline
hydrochloride (TCH) degradation experiments showed that the catalytic
activity of FeCo-ZSM-5-2:3 was much higher than those of Fe-ZSM-5
and Co-ZSM-5. In addition, the influences of catalyst dosage, PMS
concentration, reaction temperature, initial pH, and coexisting ions
on TCH removal were systematically investigated in this paper. Density
functional theory calculations indicated that Co was the main active
site for PMS adsorption, and Fe increased the area of Co’s
positive potential mapped to the electron cloud. The Fe–Co
bimetallic doping increased the area of positive potential mapped
to the electron cloud and benefited the adsorption of PMS on the catalyst
surface, which revealed the synergistic mechanism of bimetals. Electron
paramagnetic resonance spectra and quenching experiments showed that
sulfate radicals, singlet oxygen, and hydroxyl radicals were involved
in the degradation of TCH. Furthermore, liquid chromatography–mass
spectrometry was conducted to propose possible degradation pathways.
This work provides certain guiding significance in understanding the
synergistic effect of heterogeneous catalysts for tetracycline wastewater
treatment.