4.7 Article

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

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 429, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132245

Keywords

Single-atom; Co-N-3 sites; Peroxymonosulfate; Non-radical reaction; Electron-transfer

Funding

  1. Natural Science Foundation of China [52160001, 51908213, 61872141]
  2. Initial Scientific Research Foundation of Overseas High-level Talents of Harbin Institute of Technology (Shenzhen) [FA11409005]
  3. Key Research Projects of Jiangxi Province [20202BBGL73080]
  4. Program of Major Disciplines, Academic and Technical Leaders of Jiangxi Province [20204BCJL23038]
  5. Natural Science Foundation of Jiangxi Province [20192BCD40013]
  6. State Key Laboratory of Pollution Control and Resource Reuse Foundation [PCRRF19015]

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This study presents a novel biomass carbon-based catalyst capable of efficiently degrading organic pollutants like chloroquine phosphate in contaminated water. The catalyst also showed excellent efficiency in the oxidative degradation of various organic pollutants, offering a new avenue for efficient degradation of organic pollutants.
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-N-3 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 (O-1(2)) played a negligible role. The density functional theory (DFT) calculations and experimental results showed that Co-N-3 site served as the main active site for PMS activation. In addition, SA CoN-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.

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