Engineering single-atom Fe-Pyridine N-4 sites to boost peroxymonosulfate activation for antibiotic degradation in a wide pH range
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作者
Xu, Xuyang; Zhan, Fei; Pan, Jiaqi; Zhou, Lei; Su, Linghui; Cen, Wanglai; Li, Wei; Tian, Chengcheng
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刊物名称
CHEMOSPHERE
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年、卷、文献号
2022, 294, 0045-6535
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关键词
Xu, Xuyang; Zhan, Fei; Pan, Jiaqi; Zhou, Lei; Su, Linghui; Cen, Wanglai; Li, Wei; Tian, Chengcheng
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摘要
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 (O-1(2)) by regulating the Fe active sites in this study. Fe single atoms loaded on nitrogen-doped porous carbon (Fe-SA-CN) catalysts were synthesized using a cage encapsulation method and compared to Fe-nanoparticle-loaded catalysts. It was discovered that Fe-SA-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 N-4) was involved in the production of O-1(2) 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.