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

Xuyang Xu; Fei Zhan; Jiaqi Pan; Lei Zhou; Linghui Su; Wanglai Cen; Wei Li; Chengcheng Tian

doi:10.1016/j.chemosphere.2022.133735

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

Chemosphere. 2022 May:294:133735. doi: 10.1016/j.chemosphere.2022.133735. Epub 2022 Jan 24.

Authors

Xuyang Xu¹, Fei Zhan², Jiaqi Pan¹, Lei Zhou³, Linghui Su⁴, Wanglai Cen⁴, Wei Li⁵, Chengcheng Tian⁶

Affiliations

¹ National Engineering Laboratory for Industrial Wastewater Treatment, East China University of Science and Technology, Shanghai, 200237, PR China.
² Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, PR China; Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
³ State Environmental Protection Key Lab of Environmental Risk Assessment and Control on Chemical Processes, School of Resources & Environmental Engineering, East China University of Science and Technology, Shanghai, 200237, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, PR China. Electronic address: zhoulei@ecust.edu.cn.
⁴ Institute of New Energy and Low-Carbon Technology, National Engineering Research Center for Flue Gas Desulfurization, Sichuan University, Chengdu, 610207, PR China.
⁵ National Engineering Laboratory for Industrial Wastewater Treatment, East China University of Science and Technology, Shanghai, 200237, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, PR China.
⁶ National Engineering Laboratory for Industrial Wastewater Treatment, East China University of Science and Technology, Shanghai, 200237, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, PR China. Electronic address: cctian@ecust.edu.cn.

PMID: 35085615
DOI: 10.1016/j.chemosphere.2022.133735

Abstract

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 (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 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.

Keywords: Fe-pyridine N(4); Fenton-like process; PMS; Single Fe atom; Singlet oxygen.

MeSH terms

Anti-Bacterial Agents
Hydrogen-Ion Concentration
Iron*
Peroxides*
Pyridines

Substances

Anti-Bacterial Agents
Peroxides
Pyridines
peroxymonosulfate
Iron