Abstract: The Fenton-like process shows promising potential to generate reactive oxygen species for the remediation of increasingly environmental pollutants. However, the slow development of high-activity catalysts with strong stability and low leaching of metal ions has greatly inhibited scale-up application of this technology. Here, cobalt (Co)/nitrogen (N) atom co-curved carbon nanorod (CoNC) containing highly uniform CoN_x active sites is developed as a Fenton-like catalyst for the effective catalytic oxidation of various organics via peroxymonosulfate (PMS) activation with high stability. As confirmed by the experimental results, singlet oxygen (¹O₂) is the dominant active species for the degradation of the organics, with a proportion of 100%. Furthermore, density functional theory calculations indicate that CoN₂C₂ is the most effective ligand structure with more negative adsorption energy for PMS and the shortest length Co-O bond, while the most reasonable generation pathway for ¹O₂ was CoN₂C₂-PMS → CoN₂C₂-OH* → 2O* → ¹O₂. Further studies demonstrate that the electron can be transferred from the highest occupied molecular orbitals of the organics to the lowest unoccupied molecular orbitals of the PMS via CoN₂C₂ action. In addition, the CoNC presents strong resistance to inorganic ions and natural organic matter in the Fenton-like catalysis process. The presence of CoN₂C₂ active centre can significantly shorten the migration distance of the ¹O₂ generated from PMS activation, which further enhances the Fenton-like catalytic activity in terms of mineralising various organic contaminants with high efficiency over a wide pH range.

Key words: Non-radical pathway, Singlet oxygen, Co/N co-carved carbon nanorod, Fenton-like catalysis