Engineering single-atom Fe-Pyridine N4 sites to boost peroxymonosulfate activation for antibiotic degradation in a wide pH range

Single-atom Fe catalysts have shown great potential for Fenton-like technology in organic pollutant decomposition. However, the underlying reaction pathway and the identification of Fe active sites capable of activating peroxymonosulfate (PMS) across a wide pH range remain unknown. We presented a no...

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Bibliographic Details
Published in:Chemosphere (Oxford) 2022-05, Vol.294, p.133735-133735, Article 133735
Main Authors: Xu, Xuyang, Zhan, Fei, Pan, Jiaqi, Zhou, Lei, Su, Linghui, Cen, Wanglai, Li, Wei, Tian, Chengcheng
Format: Article
Language:English
Subjects:
Fe-pyridine N4
Fenton-like process
PMS
Single Fe atom
Singlet oxygen
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Summary:Single-atom Fe catalysts have shown great potential for Fenton-like technology in organic pollutant decomposition. However, the underlying reaction pathway and the identification of Fe active sites capable of activating peroxymonosulfate (PMS) across a wide pH range remain unknown. We presented a novel strategy for deciphering the production of singlet oxygen (1O2) by regulating the Fe active sites in this study. Fe single atoms loaded on nitrogen-doped porous carbon (FeSA-CN) catalysts were synthesized using a cage encapsulation method and compared to Fe-nanoparticle-loaded catalysts. It was discovered that FeSA-CN catalysts served as efficient PMS activators for pollutant decomposition over a wide pH range. Several analytical measurements and density functional theory calculations revealed that the pyridinic N-ligated Fe single atom (Fe-pyridine N4) was involved in the production of 1O2 by the binding of two PMS ions, resulting in an excellent catalytic performance for PMS adsorption/activation. This work has the potential to not only improve the understanding of nonradical reaction pathway but to also provide a generalizable method for producing highly stable PMS activators with high activity for practical wastewater treatment. [Display omitted] •Efficient singlet oxygen formation was achieved by regulating the Fe active sites.•FeSA-CN exhibited high PMS activation activity and stability over a wide pH range.•Fe-pyridine N4 site was responsible for excellent catalytic performance.
ISSN:0045-6535
1879-1298
DOI:10.1016/j.chemosphere.2022.133735