期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 55, 期 2, 页码 1260-1269出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.0c06825
关键词
electro-Fenton; heterogeneous Fenton; FeNx sites; H2O2; Fe3C particles; electrochemical catalysis
资金
- Natural Science Foundation of China [NSFC21477165]
- Fundamental Research Funds for the Central Universities
- South-Central University for Nationalities [CZP20005, CZQ17004]
The Fe-based catalyst with core-shell structure showed significant performance in degrading chlorophenols under various conditions while maintaining low levels of leached iron. Experimental results confirmed center dot OH as the key reactive species, with Fe-IV playing a role in neutral conditions.
Heterogeneous electro-Fenton (HEF) reaction has been considered as a promising process for real effluent treatments. However, the design of effective catalysts for simultaneous H2O2 generation and activation to achieve bifunctional catalysis for O-2 toward center dot OH production remains a challenge. Herein, a core-shell structural Fe-based catalyst (FeNC@C), with Fe3C and FeN nanoparticles encapsulated by porous graphitic layers, was synthesized and employed in a HEF system. The FeNC@C catalyst presented a significant performance in degradation of various chlorophenols at various conditions with an extremely low level of leached iron. Electron spin resonance and radical scavenging revealed that center dot OH was the key reactive species and Fe-IV would play a role at neutral conditions. Experimental and density function theory calculation revealed the dominated role of Fe3C in H2O2 generation and the positive effect of FeNx sites on H2O2 activation to form center dot OH. Meanwhile, FeNC@C was proved to be less pH dependence, high stability, and well-recycled materials for practical application in wastewater purification.
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