<p>Magnetic iron oxide (Fe<sub>3</sub>O<sub>4</sub>) nanoparticles are widely recognized for their potential in environmental remediation owing to their excellent magnetic properties, chemical stability, and recyclability. However, their standalone photocatalytic performance remains limited due to rapid charge carrier recombination, particle agglomeration, and low surface activity. In this study, Fe<sub>3</sub>O<sub>4</sub> was coupled with graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) to form a Fe<sub>3</sub>O<sub>4</sub>/g-C<sub>3</sub>N<sub>4</sub> ceramics nanocomposite, synthesized through a high-energy ball-milling process. XRD, FTIR, XPS, BET, Raman measurements were performed to demonstrate that Fe<sub>3</sub>O<sub>4</sub> and g-C<sub>3</sub>N<sub>4</sub> were successfully integrated to make a stable heterojunction. The incorporation of Fe<sub>3</sub>O<sub>4</sub> reduced the bandgap energy of g-C<sub>3</sub>N<sub>4</sub> from 2.81&#xa0;eV to 2.12&#xa0;eV, enhancing visible-light absorption. BET analysis revealed a surface area of 49.79 m<sup>2</sup>/g and mesoporous structure, supporting improved adsorption and charge transfer. Raman shift of T<sub>12g</sub> and E<sub>g</sub> modes also confirmed that there was a high interfacial interaction between Fe<sub>3</sub>O<sub>4</sub> and g-C<sub>3</sub>N<sub>4</sub>. Under visible-light irradiation, the Fe<sub>3</sub>O/g-C3N ceramics nanocomposite achieved 95% degradation of malachite green (MG) within 60&#xa0;min. The addition of H2O2 further promoted degradation through a photo-Fenton-like mechanism. Scavenger experiments also confirmed that <sup>•</sup>OH and <i>h</i><sup><i>+</i></sup> were the main reactive species, which validated the synergistic photocatalytic/photo-Fenton pathway. Furthermore, kinetic analysis followed pseudo-first-order behavior consistent with the Langmuir–Hinshelwood model. The material also demonstrated excellent stability, magnetic separability, and reusability across multiple cycles. The novelty of this work lies in the development of a magnetically recoverable Fe<sub>3</sub>O<sub>4</sub>/g-C<sub>3</sub>N<sub>4</sub> ceramic nanocomposite via a green, solvent-free ball-milling approach, integrating visible-light photocatalysis with Fenton-like activity for sustainable wastewater treatment.</p>

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Photo-activated Fenton-like degradation of Malachite Green using Fe₃O₄/g-C₃N₄ Ceramics Nanocomposites: Kinetics, Stability, and Mechanistic Insights

  • Mohd Imran,
  • Ahmad Zuhairi Abdullah,
  • Mohammad Ehtisham Khan,
  • Fazlurrahman Khan,
  • Kahkashan Anjum,
  • Syed Kashif Ali,
  • Abdullah Ali Alamri,
  • Sally Mostafa Khadrawy

摘要

Magnetic iron oxide (Fe3O4) nanoparticles are widely recognized for their potential in environmental remediation owing to their excellent magnetic properties, chemical stability, and recyclability. However, their standalone photocatalytic performance remains limited due to rapid charge carrier recombination, particle agglomeration, and low surface activity. In this study, Fe3O4 was coupled with graphitic carbon nitride (g-C3N4) to form a Fe3O4/g-C3N4 ceramics nanocomposite, synthesized through a high-energy ball-milling process. XRD, FTIR, XPS, BET, Raman measurements were performed to demonstrate that Fe3O4 and g-C3N4 were successfully integrated to make a stable heterojunction. The incorporation of Fe3O4 reduced the bandgap energy of g-C3N4 from 2.81 eV to 2.12 eV, enhancing visible-light absorption. BET analysis revealed a surface area of 49.79 m2/g and mesoporous structure, supporting improved adsorption and charge transfer. Raman shift of T12g and Eg modes also confirmed that there was a high interfacial interaction between Fe3O4 and g-C3N4. Under visible-light irradiation, the Fe3O/g-C3N ceramics nanocomposite achieved 95% degradation of malachite green (MG) within 60 min. The addition of H2O2 further promoted degradation through a photo-Fenton-like mechanism. Scavenger experiments also confirmed that OH and h+ were the main reactive species, which validated the synergistic photocatalytic/photo-Fenton pathway. Furthermore, kinetic analysis followed pseudo-first-order behavior consistent with the Langmuir–Hinshelwood model. The material also demonstrated excellent stability, magnetic separability, and reusability across multiple cycles. The novelty of this work lies in the development of a magnetically recoverable Fe3O4/g-C3N4 ceramic nanocomposite via a green, solvent-free ball-milling approach, integrating visible-light photocatalysis with Fenton-like activity for sustainable wastewater treatment.