<p>Iron-based spinel oxides, with excellent catalytic activity and stability, hold promising potential in the photo-Fenton degradation of organic pollutants. In this study, (Fe<sub>0.2</sub>Co<sub>0.2</sub>Ni<sub>0.2</sub>Cu<sub>0.2</sub>Mn<sub>0.2</sub>)Fe<sub>2</sub>O<sub>4</sub> was prepared via the solution combustion method. Multiple characterization techniques confirmed the good stability and morphology of (Fe<sub>0.2</sub>Co<sub>0.2</sub>Ni<sub>0.2</sub>Cu<sub>0.2</sub>Mn<sub>0.2</sub>)Fe<sub>2</sub>O<sub>4</sub>. It exhibited high-entropy oxide properties, making it suitable as a photo-Fenton catalyst for the efficient degradation of oxytetracycline hydrochloride (OTC-HCl). Under visible light (Vis) with 10 mM H<sub>2</sub>O<sub>2</sub>, 0.06 g/L OTC-HCl, and pH 4.0, the catalyst achieved a degradation efficiency of 92.9%. In the photo-Fenton system, the utilization rate of H<sub>2</sub>O<sub>2</sub> (calculated as the ratio of the degradation amount of OTC-HCl to the consumption amount of H<sub>2</sub>O<sub>2</sub>) was 34.5, which is 8.3 times higher than that of pure H<sub>2</sub>O<sub>2</sub> (4.2). The catalyst showed good acid–base adaptability, achieving OTC-HCl removal rates exceeding 92.0% across a pH range of 3–11, with a reaction rate constant of 0.08 min<sup>−1</sup> at pH 11. Free-radical capture experiments showed that (Fe<sub>0.2</sub>Co<sub>0.2</sub>Ni<sub>0.2</sub>Cu<sub>0.2</sub>Mn<sub>0.2</sub>)Fe<sub>2</sub>O<sub>4</sub> catalyzed H<sub>2</sub>O<sub>2</sub> to generate <b>·</b>OH, <b>·</b>O<sub>2</sub><sup>−</sup>, and e<sup>−</sup>, which are the main free radicals involved in the degradation of OTC-HCl. In summary, (Fe<sub>0.2</sub>Co<sub>0.2</sub>Ni<sub>0.2</sub>Cu<sub>0.2</sub>Mn<sub>0.2</sub>)Fe<sub>2</sub>O<sub>4</sub> not only addresses the issue of low H<sub>2</sub>O<sub>2</sub> utilization in traditional photo-Fenton systems but also catalyzes the generation of H<sub>2</sub>O<sub>2</sub> under light conditions. Thus, it can serve as an excellent photo-Fenton catalyst for OTC-HCl degradation.</p> Graphical Abstract <p></p>

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Synthesis of (Fe0.2Co0.2Ni0.2Cu0.2Mn0.2)Fe2O4 High Entropy Spinel Oxide for Photo-Fenton Degradation of Oxytetracycline Hydrochloride Over a Wide pH Range

  • Yuxin Gan,
  • Dan Liu,
  • Zhipu Wang,
  • Ge Huang,
  • Rumei Ze,
  • Xiaohong Wang,
  • Jiabin Zhou

摘要

Iron-based spinel oxides, with excellent catalytic activity and stability, hold promising potential in the photo-Fenton degradation of organic pollutants. In this study, (Fe0.2Co0.2Ni0.2Cu0.2Mn0.2)Fe2O4 was prepared via the solution combustion method. Multiple characterization techniques confirmed the good stability and morphology of (Fe0.2Co0.2Ni0.2Cu0.2Mn0.2)Fe2O4. It exhibited high-entropy oxide properties, making it suitable as a photo-Fenton catalyst for the efficient degradation of oxytetracycline hydrochloride (OTC-HCl). Under visible light (Vis) with 10 mM H2O2, 0.06 g/L OTC-HCl, and pH 4.0, the catalyst achieved a degradation efficiency of 92.9%. In the photo-Fenton system, the utilization rate of H2O2 (calculated as the ratio of the degradation amount of OTC-HCl to the consumption amount of H2O2) was 34.5, which is 8.3 times higher than that of pure H2O2 (4.2). The catalyst showed good acid–base adaptability, achieving OTC-HCl removal rates exceeding 92.0% across a pH range of 3–11, with a reaction rate constant of 0.08 min−1 at pH 11. Free-radical capture experiments showed that (Fe0.2Co0.2Ni0.2Cu0.2Mn0.2)Fe2O4 catalyzed H2O2 to generate ·OH, ·O2, and e, which are the main free radicals involved in the degradation of OTC-HCl. In summary, (Fe0.2Co0.2Ni0.2Cu0.2Mn0.2)Fe2O4 not only addresses the issue of low H2O2 utilization in traditional photo-Fenton systems but also catalyzes the generation of H2O2 under light conditions. Thus, it can serve as an excellent photo-Fenton catalyst for OTC-HCl degradation.

Graphical Abstract