Calcination temperature regulates non-radical pathways of peroxymonosulfate activation via carbon catalysts doped by iron and nitrogen

作者：Wang, Yue; Lin, Yan; Yang, Chunping^*; Wu, Shaohua^*; Fu, Xintao; Li, Xiang

来源：Chemical Engineering Journal, 2023, 451: 138468.

DOI：10.1016/j.cej.2022.138468

• Singlet oxygen
• High-valent iron-oxo species
• Peroxymonosulfate
• Active site
• Advanced oxidation

Switching the reaction routes between radical pathways and non-radical ones in peroxymonosulfate (PMS) activation has attracted much interest, however, the regulation between non-radical pathways remains elusive. Herein, we reported the regulation of the dominant non-radical routes in PMS activation with carbon catalysts doped by iron and nitrogen (Fe-N/C) through varying the calcination temperature of conductive polymer Fepolyaniline complexes. High calcination temperatures ranging from 300 degrees C to 900 degrees C boosted the catalytic activity and surprisingly switched the non-radical activation routes from electron transfer to singlet oxygen (1O2) and high-valent iron-oxo species (HV-Fe--O). Pyrrolic N and C--O formed at 300 degrees C accounted for the electron transfer process, while graphitic N, O-C--O, and Fe-Nx formed over 700 degrees C were key catalytic sites responsible for the production of 1O2 and HV-Fe--O. Moreover, the catalyst calcinated at 900 degrees C (900@Fe-N/C-2) maximized bisphenol A removal by 96.4% and TOC removal by 83.0%. The optimal 900@Fe-N/C-2/PMS system could work efficiently over a wide pH range or coexisting water components. This study provided a facile strategy to regulate PMS non-radical pathways for the treatment of complicated wastewater.

• 单位
  茂名学院; 南昌航空大学