In-situ synthesis of N, S co-doped hollow carbon microspheres for efficient catalytic oxidation of organic contaminants

Metal-free heteroatom doped nanocarbons are promising alternatives to the metal-based materials in catalytic ozonation for destruction of aqueous organic contaminants. In this study, N, S co-doped hollow carbon microspheres (NSCs) were synthesized from the polymerization products during persulfate wet air oxidation of benzothiazole. The contents of doped N and S as well as the structural stability were maneuvered by adjusting the subsequent N-2-annealing temperature. Compared with the prevailing single-walled carbon nanotubes, the N-2-annealed NSCs demonstrated a higher catalytic ozonation activity for benzimidazole degradation. According to the quantitative structure-activity relationship (QSAR) analysis, the synergistic effect between the graphitic N and the thiophene-S which redistributed the charge distribution of the carbon basal plane contributed to the activity enhancement of the N-2-annealed NSCs. Additionally, the hollow structure within the microspheres served as the microreactor to boost the mass transfer and reaction kinetics via the nanoconfinement effects. Quenching and electron paramagnetic resonance (EPR) tests revealed that benzimidazole degradation was dominated by the produced singlet oxygen (O-1(2)) species, while hydroxyl radicals ((OH)-O-center dot) were also generated and participated. This study puts forward a novel strategy for synthesis of heteroatom-doped nanocarbons and sheds a light on the relationship between the active sites on the doped nanocarbons and the catalytic performance. (C) 2021 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.

Automated summary

Metal-free heteroatom doped nanocarbons, such as N, S co-doped hollow carbon microspheres, have been studied as promising alternatives to metal-based materials for catalytic ozonation of aqueous organic contaminants. This study investigated the synthesis and catalytic performance of N- and S-doped hollow carbon microspheres and found that the N-2-annealed NSCs exhibited higher catalytic activity compared to single-walled carbon nanotubes. The activity enhancement was attributed to the synergistic effect between graphitic nitrogen and thiophene sulfur, as well as the nanoconfinement effects provided by the hollow structure within the microspheres.