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This research demonstrates improved fe atom density and feiv=o generation in catalysts, suggesting enhanced catalytic activity for pollutant degradation.
Fe-based single-atom catalysts display extraordinary activity in the Fenton-like reaction, but low Fe atom densities limit their overall catalytic performance. In addition, high-valent iron (as FeIV═O) plays a pivotal role due to the selective degradation of contaminants in water. However, it is rarely reported for FeIV═O generation in the H2O2-based Fenton-like process. This study confirmed that the Fe atom (Fe2+ and Fe3+) and the Fe cluster coexisted in the as-synthesized catalyst, in which the penta-coordinated Fe atom (Fe-N5) was found instead of the normal Fe-N4. The Fe content reaches 13.7 wt % in the catalyst, which is significantly higher than the normal Fe atom density (less than 5 wt %). The ratio of the Fe atom to the Fe cluster is 89.8% at the surface of the catalyst. Furthermore, FeIV═O was generated during the H2O2-based Fenton-like reaction. The density functional theory and experimental results confirm that the synergistic effect between FeN5 and the Fe cluster enhanced the catalytic activity and FeIV═O formation. The catalyst showed selective degradation for electron-rich contaminants such as tetracycline hydrochloride via the Fenton-like reaction, in which the nonradical pathway by FeIV═O dominated the degradation process.
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Li et al. (2025) studied this question.