4.7 Article

Defect modulation of MOF-derived ZnFe2O4/CNTs microcages for persulfate activation: Enhanced nonradical catalytic oxidation

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 431, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133369

Keywords

Persulfate; Non-radical activation; Electron transfer; Defective CNTs; ZnFe2O4

Funding

  1. National Natural Science Foundation of China [51978372, 51978373]
  2. National Key R&D Program of China [2019YFA0705802]

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There has been increasing interest in combining porous metal organic frameworks (MOFs) with conductive carbonaceous materials to enhance catalytic activity. In this study, a simple strategy was developed to synthesize a highly efficient and recyclable heterogeneous catalyst through the pyrolysis of MOFs as sacrificial templates. The introduction of defective sites in the carbon nanotubes (CNTs) precursor significantly improved the charge transfer capability of the composite microcages and the coordination environment of Fe centers. With the assistance of persulfate oxidants, the modulated defects in ZnFe2O4/CNTs-Ar exhibited a 17.5-fold higher reaction rate for Bisphenol A degradation compared to blank ZnFe(2)O(4) microcages. Experimental characterizations indicated that the defective CNTs facilitated the electron transfer from BPA molecules to persulfate, triggering the direct decomposition of pollutants through a non-radical oxidation pathway. This research provides a new strategy for developing high-performance MOFs-derived catalysts for wastewater treatment.
There has been growing interest in the combination of porous metal organic frameworks (MOFs)-derived ar-chitectures with conductive carbonaceous materials for the synergistically enhanced catalytic activity. Herein, we described a facile strategy to synthesize a highly efficient and recyclable heterogeneous catalyst through pyrolysis of MOFs as sacrificial templates. We found that creating defective sites in CNTs precursors exhibited significant impact on the charge transfer capability of composite microcages and the coordination environment of Fe centers. With the assistant of persulfate oxidants, ZnFe2O4/CNTs-Ar with modulated defects exhibited 17.5-fold higher kinetic reaction rate (0.35 min(-1)) than blank ZnFe(2)O(4)microcages for Bisphenol A degradation. Experimental characterizations suggested that defective CNTs played a vital role in shuttling electron from BPA molecules to persulfate, triggered the direct decomposition of pollutants via a non-radical oxidation pathway. Our research provides a new strategy to develop high-performance MOFs-derived catalysts through defect modulation for wastewater treatment.

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