4.7 Article

Two-dimensional ultrathin perforated Co3O4 nanosheets enhanced PMS-Activated selective oxidation of organic micropollutants in environmental remediation

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 427, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.131953

Keywords

Two-dimensional ultrathin nanosheets; Cobaltosic oxide; PMS activation; Selective degradation

Funding

  1. National Natural Science Foundation of China [22006022]
  2. One Hundred Youth Science and Technology Plan Guangdong University of Technology, China [220413320]
  3. European Union's Horizon 2020 research and innovation programme under the Marie Skodowska-Curie Grant [838593]
  4. Marie Curie Actions (MSCA) [838593] Funding Source: Marie Curie Actions (MSCA)

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A two-dimensional ultrathin perforated Co3O4 nanosheet was designed by wet-chemical synthesis to activate PMS for efficient selective oxidation, showing a high degradation efficiency of BPA. The enhanced catalytic performance can be attributed to its large surface area and pore diameter in porous 2D structure, as well as the strong electrostatic attraction with PMS.
Here a two-dimensional (2D) ultrathin perforated Co3O4 nanosheet is rationally designed by a wet-chemical synthesis to activate peroxymonosulfate (PMS) for efficient selective oxidation. And the physicochemical properties of catalyst were investigated by series of techniques. The Co3O4 nanosheets achieved a 98.0% degradation efficiency of bisphenol A (BPA) within 30 min, showing a 4 times higher kinetic constant (0.112 min-1) and 5 times lower Co2+ leakage (6.5 mu g/L), than commercial Co3O4 microspheres. The great enhancement in catalytic performance was ascribed to the large surface area and pore diameter in porous 2D structure, as well as the strong electrostatic attraction with PMS. Moreover, the influence of several parameters such as initial pH, temperatures, humic acids and inorganic anions in the system on the remaval of BPA were systematically studied. Since sulfate radicals (SO4 center dot- ) were proved to be the primary reactive oxygen species by EPR measurements and quenching experiments, the PMS/Co3O4 nanosheets exhibits a highly selective oxidation on aromatics with electron donating groups (i.e., -OH and -CH3), while a relatively low value for organics with electronwithdrawing groups (e.g., -NO2 and -COOH). A high ionization potential threshold was determined to be greater than 9.39 eV, corresponding to a high oxidation ability to react with the organics. Finally, possible degradation pathways were proposed based on twenty intermediate products determined from mass spectrometry.

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