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

引用

Chinese Chemical Letters 2022年第3期33卷 1298-1302页

作者： Yongbing Xie Ya Liu Yujie Yao Yanchun shi Binran Zhao Yuxian Wang state Key Laboratory of Vanadium and Titanium Resources comprehensive Utilization Panzhihua 617000China CAs Key Laboratory of Green Process&Engineering Beijing Engineering Research Center of Process Pollution ControlInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China state Key Laboratory of Heavy Oil Processing State Key Laboratory of Petroleum Pollution ControlChina University of Petroleum-BeijingBeijing 102249China school of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia school of Chemical Engineering Northwest UniversityXi'an 710069China

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 (^(1)O_(2)) 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.

关键词： Metal-free catalysis Hollow carbon microspheres n,s co-doping Catalytic ozonation singlet oxygen(1O_(2))

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