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Spin-State-Modulated Interfacial Fe2+ in Solid-Solution Heterostructures Promotes H2O2 Selectivity and Electro-Fenton
Jitao Li1, Sichen Huo2, Wei Wang1
1School of Civil Engineering, Heilongjiang Institute of Technology, Harbin 150050, China.
ACS Applied Materials & Interfaces
|May 7, 2026
Summary
This study introduces a novel CoFe solid solution/Fe3O4 catalyst for efficient electro-Fenton (EF) processes. The engineered catalyst selectively generates hydrogen peroxide (H2O2) and hydroxyl radicals (•OH) for effective antibiotic wastewater treatment.
Area of Science:
- Materials Science
- Catalysis
- Environmental Chemistry
Background:
- Heterogeneous electro-Fenton (EF) catalysis faces challenges in selective H2O2 generation and •OH production due to poor oxygen reduction reaction (ORR) selectivity and stability.
- Achieving efficient pollutant degradation in wastewater treatment requires catalysts with high selectivity and stability.
Purpose of the Study:
- To develop an efficient heterogeneous catalyst for electro-Fenton (EF) processes by engineering the spin-state of iron ions at the interface.
- To improve the selectivity of the oxygen reduction reaction (ORR) towards H2O2 generation and enhance the production of hydroxyl radicals (•OH).
- To investigate the catalyst's performance in degrading tetracycline and assess its environmental safety.
Main Methods:
- Constructed CoFe solid solutions/Fe3O4 heterostructures (CoFe_ss/Fe3O4) using controlled cobalt doping.
- Investigated the interfacial spin-state engineering strategy by analyzing the Fe2+ spin-state transition at the heterointerface.
- Evaluated the catalyst's performance in tetracycline degradation and assessed the reactive oxygen species involved.
Main Results:
- The CoFe_ss/Fe3O4 catalyst exhibited a 2-electron ORR pathway with 75.9% H2O2 selectivity.
- Co0.1Fe_ss/Fe3O4 achieved 95.0% tetracycline removal within 60 min, outperforming the undoped catalyst.
- Degradation was primarily driven by •OH radicals, with synergistic contributions from •O2- and 1O2, leading to low toxicity of intermediates.
Conclusions:
- Heterometallic doping and interfacial spin-state engineering are effective strategies for designing efficient EF catalysts.
- The developed CoFe_ss/Fe3O4 catalyst shows promise for treating antibiotic wastewater with high efficiency and environmental safety.
- This approach provides insights for developing advanced catalysts for environmental remediation applications.
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