Citation: Yongbing Xie, Ya Liu, Yujie Yao, Yanchun Shi, Binran Zhao, Yuxian Wang. In-situ synthesis of N, S co-doped hollow carbon microspheres for efficient catalytic oxidation of organic contaminants[J]. Chinese Chemical Letters, ;2022, 33(3): 1298-1302. doi: 10.1016/j.cclet.2021.07.055 shu

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

Yongbing Xie ^{a, b} ,
Ya Liu ^{c, d} ,
Yujie Yao ^{b, e} ,
Yanchun Shi ^b ,
Binran Zhao ^{e, *,} ,
Yuxian Wang ^{c, *,}

a.
State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization, Panzhihua 617000, China
b.
CAS Key Laboratory of Green Process & Engineering, Beijing Engineering Research Center of Process Pollution Control, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
c.
State Key Laboratory of Heavy Oil Processing, State Key Laboratory of Petroleum Pollution Control, China University of Petroleum-Beijing, Beijing 102249, China
d.
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia
e.
School of Chemical Engineering, Northwest University, Xi'an 710069, China

zhaobr@nwu.edu.cn

wang@cup.edu.cn

Received Date: 14 May 2021
Revised Date: 5 July 2021
Accepted Date: 24 July 2021
Available Online: 31 July 2021
Fund Project: the financial supports from the National Natural Science Foundation of China 21978324Tianjin Municipal Science and Technology Bureau 18YFYSZ00170Beijing Natural Science Foundation 8192039Science Foundation of China University of Petroleum, Beijing 2462020YXZZ034

Figures(5)

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 N₂-annealing temperature. Compared with the prevailing single-walled carbon nanotubes, the N₂-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 N₂-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 (¹O₂) species, while hydroxyl radicals (^·OH) 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.
- Metal-free catalysis,
- Hollow carbon microspheres,
- N, S co-doping,
- Catalytic ozonation,
- Singlet oxygen (¹O₂)
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