4.7 Article

Singlet oxygen-dominated transformation of oxytetracycline by peroxymonosulfate with CoAl-LDH modified hierarchical porous ceramics: Toxicity assessment

期刊

CHEMICAL ENGINEERING JOURNAL
卷 436, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135199

关键词

Peroxymonosulfate; CoAl LDH; Singlet oxygen; Transformation products; Toxicity assessment; 3D printed impeller-agitator

资金

  1. National Natural Science Foundation of China [21304040]
  2. Fundamental Research Funds for the Central Universities [lzujbky-2020-68]

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In this study, CoAl-LDH modified 3D printed hierarchical porous ceramics were used to efficiently activate peroxymonosulfate for the degradation of oxytetracycline. The results showed high removal efficiency and transformation into less toxic by-products. The study provides a new approach to design functional devices and treat bio-refractive contaminants.
Singlet oxygen (1O2) dominated advanced oxidation processes have gained much attention due to their ability to transform or even detoxify organic pollutants. Herein we report that CoAl-LDH modified 3D printed hierarchical porous ceramics (3DP-HPC@CoAl-LDH) were able to efficiently activate peroxymonosulfate to degrade oxytet-racycline (OTC) at pH 6.2 (over 99% removal in 30 min) and transform it into less toxic by-products. Cl- and natural organic matter showed an inhibitory effect on OTC degradation. Quenching experiments and ESR results identified the main contribution of 1O2 to OTC oxidation besides SO4 center dot-& nbsp;& nbsp;, O-2(center dot-)- and & BULL;OH. Several possible pathways of OTC degradation were proposed based on the by-products detected using LC-MS. T.E.S.T calculation based on quantitative structure-activity relationships (QSARs) revealed detoxification of transformation products. Flow cytometry method was applied to quantify the cytotoxic effects of the reaction solution including the degradation products at various reaction times. Density functional theory simulation suggested that the strong electronic interaction between Co (II) and PMS allowed the 3DP-HPC@CoAl-LDH to effectively adsorb HSO5- and split the O-O bond. Moreover, the 3DP-HPC@CoAl-LDH can be separated directly from water and reused with a degra-dation efficiency of more than 83% after 11 cycles, demonstrating high recyclability and sustainable catalytic efficiency. Furthermore, a 3D printed impeller-agitator was fabricated and evaluated for potential practical application. The strategy proposed in this study may provide alternative approach to design functional devices as PMS activators and treat bio-refractive contaminants for practical applications.

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