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Activation of peroxymonosulfate by single atom Co-N-C catalysts for high-efficient removal of chloroquine phosphate via non-radical pathways: Electron-transfer mechanism

Peng, Xiaoming ; Wu, Jianqun ; Zhao, Zilong ; Wang, Xing ; Dai, Hongling ; Wei, Yang ; Xu, Gaoping ; Hu, Fengping

Chemical engineering journal (Lausanne, Switzerland : 1996), 2022-02, Vol.429, p.132245, Article 132245 [Periódico revisado por pares]

Elsevier B.V

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  • Título:
    Activation of peroxymonosulfate by single atom Co-N-C catalysts for high-efficient removal of chloroquine phosphate via non-radical pathways: Electron-transfer mechanism
  • Autor: Peng, Xiaoming ; Wu, Jianqun ; Zhao, Zilong ; Wang, Xing ; Dai, Hongling ; Wei, Yang ; Xu, Gaoping ; Hu, Fengping
  • Assuntos: Co–N3 sites ; Electron-transfer ; Non-radical reaction ; Peroxymonosulfate ; Single-atom
  • É parte de: Chemical engineering journal (Lausanne, Switzerland : 1996), 2022-02, Vol.429, p.132245, Article 132245
  • Descrição: •Co-N-C SACs with Co-Nx sites was successfully synthesized by facile method.•SA Co-N-C(30) exhibited an excellent catalytic performance for PMS activation.•Experiments and DFT calculations demonstrated Co-N3 was optimum active site.•The electron-transfer was regarded as the dominated reactive pathway for CQP degradation. Chloroquine phosphate (CQP) has played a role in the remission of COVID-19, but its large use will undoubtedly pollute the water. Herein, we have designed biomass carbon-based catalysts with anchoring sites for single cobalt atoms in a defined Co-N3 coordination structure (SA Co-N-C(30)). A peroxymonosulfate (PMS) activation system employing the SA Co-N-C(30) as a high-efficiency catalyst was demonstrated, which can efficiently degrade CQP in a wide pH range (3–11). The electron-transfer was proposed as the dominant non-radical pathway for CQP degradation in SA Co-N-C(30)/PMS system by electrochemical studies and quenching experiments, and the generated singlet oxygen (1O2) played a negligible role. The density functional theory (DFT) calculations and experimental results showed that Co-N3 site served as the main active site for PMS activation. In addition, SA Co-N-C(30)/PMS system had excellent efficiencies in oxidative degradation of various organic pollutants. This work opens up a new avenue to efficient degradation of organic pollutants.
  • Editor: Elsevier B.V
  • Idioma: Inglês
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  • Realização: ABCD-USP USP   Logos de Redes Sociais: Freepik

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