化学
单线态氧
吡啶
吸附
降级(电信)
分解
光化学
无机化学
催化作用
物理化学
氧气
有机化学
电信
计算机科学
作者
Xuyang Xu,Fei Zhan,Jiaqi Pan,Lei Zhou,Linghui Su,Wanglai Cen,Wei Li,Chengcheng Tian
出处
期刊:Chemosphere
[Elsevier]
日期:2022-05-01
卷期号:294: 133735-133735
被引量:29
标识
DOI:10.1016/j.chemosphere.2022.133735
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 (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.
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