文献类型：期刊文献

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

作者：Xu, Xuyang[1];Zhan, Fei[5,6];Pan, Jiaqi[1];Zhou, Lei[2,3];Su, Linghui[4];Cen, Wanglai[4];Li, Wei[1,3];Tian, Chengcheng[1,3]

机构：[1]East China Univ Sci & Technol, Natl Engn Lab Ind Wastewater Treatment, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Resources & Environm Engn, State Environm Protect Key Lab Environm Risk Asse, Shanghai 200237, Peoples R China;[3]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;[4]Sichuan Univ, Natl Engn Res Ctr Flue Gas Desulfurizat, Inst New Energy & Low Carbon Technol, Chengdu 610207, Peoples R China;[5]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[6]Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China

年份：2022

卷号：294

外文期刊名：CHEMOSPHERE

收录：;EI(收录号：20220411536601);WOS:【SCI-EXPANDED(收录号:WOS:000760137300003)】；

基金：This study was supported financially by the key project of the Na-tional Natural Science Foundation of China (52030001) . HAADF-STEM data were provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center. XAFS data were collected at the Shanghai Synchrotron Radiation Facility in Shanghai Advanced Research Institute, Chinese Academy of Sciences.

语种：英文

外文关键词：Single Fe atom; PMS; Singlet oxygen; Fe-pyridine N-4; Fenton-like process

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.