4.7 Article

Synergistically enhanced activation of persulfate for efficient oxidation of organic contaminants using a microscale zero-valent aluminum/Fe-bearing clay composite

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 433, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133682

Keywords

Zero-valent aluminum; Fe-bearing clay mineral; Persulfate; Activation; Oxidation of organic contaminants; Synergistic mechanisms

Funding

  1. National Natural Science Foundation of China [42061144014, 51978325]
  2. Quanzhou Bay Plan Introduced High-level Talents Team Project [2021CT001]

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Sulfate radical-based advanced oxidation processes have gained attention in contaminated water treatment. Microscale zero-valent aluminum (mZVAl) is an excellent electron donor and can activate persulfate (PS). However, the natural oxide layer of mZVAl hinders electron transfer. In this study, a composite material consisting of mZVAl and Fe-bearing clay (mZVAl-NaNAu-2) was obtained through ball milling and showed excellent efficiency in degrading various organic contaminants in water.
Sulfate radical-based advanced oxidation processes have received increasing attention in contaminated water treatment. As an excellent electron donor, microscale zero-valent aluminum (mZVAl) is a promising persulfate (PS) activator. However, the natural oxide layer of mZVAl impedes electron transfer from the core metal. Herein, a composite comprising mZVAl and Fe-bearing clay (mZVAl-NaNAu-2) was obtained through the simple ball milling (BM), which synergistically activates PS for the efficient degradation of various organic contaminants, such as 4-chlorophenol, benzoic acid, nitrobenzene, phenol, and ofloxacin, in water. The sulfate radicals and hydroxyl radicals were the main reactive species but Fe(IV) was minor in this reaction. The BM can cause fracture of the mZVAl powder and promote exposure of the fresh Al-0 surface. Various Fe species in mZVAl-NaNAu-2 at different reaction times were evaluated by extraction experiments, Mo & BULL;ssbauer and XPS spectra. Approximately 47.0% of structural Fe(III) was reduced to Fe(II) after BM. The dissolved Fe(II) and structural trioctahedral Fe(II)Fe(II)-Fe(II) entities were mainly responsible for the homogeneous and heterogeneous activation of PS, and corroded mZVAl acted as an electron pool to regenerate the aforementioned Fe(II) species continuously. The mZVAl-NaNAu-2/PS system also presented certain resistance to a natural organic matter and some anions, such as Cl- and NO -3. This study provided a new strategy for the efficient removal of organic contaminants from water and also solved the bottleneck of mZVAl in applications due to its dense oxide film.

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