<p>Developing advanced and eco-friendly materials for wastewater treatment is critical to addressing global water pollution. In this study, a novel chitosan–UiO-66 metal–organic framework (MOF)–TiO<sub>2</sub> (CS-UiO-66-TiO<sub>2</sub>) hybrid composite was synthesized and evaluated for the removal of Auramine O (AO) via adsorption and photocatalysis. The hybrid composite exhibited a maximum adsorption capacity of 368.8&#xa0;mg/g and a removal efficiency of 98.44% under optimal conditions (pH 6, 260&#xa0;min, and 160&#xa0;mg/L AO). Comprehensive characterization, including scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) surface area analysis, and thermogravimetric analysis (TGA), provided conclusive evidence that UiO-66 MOF and TiO<sub>2</sub> were successfully integrated into the chitosan matrix, enhancing structural integrity and chemical reactivity. BET analysis revealed a high surface area of 786.84&#xa0;m<sup>2</sup>/g, contributing to enhanced adsorption performance. The adsorption process was best described by the pseudo-second-order (PSO) kinetic model, demonstrating excellent agreement with experimental data in both linear (R<sup>2</sup> = 0.998) and non-linear (R<sup>2</sup> = 0.999) forms. Additionally, the Freundlich isotherm provided the best fit for the equilibrium data, with correlation coefficients of R<sup>2</sup> = 0.999 (linear) and R<sup>2</sup> = 0.998 (non-linear), indicating adsorption on a heterogeneous surface with multiple binding sites. Thermodynamic analysis confirmed the process was spontaneous and endothermic, with Gibbs free energy change (ΔG) ranging from −&#xa0;5.43 to −&#xa0;9.61&#xa0;kJ/mol (298.15–338.15&#xa0;K), enthalpy change (ΔH) of + 80.85&#xa0;kJ/mol, and entropy change (ΔS) of + 37.85&#xa0;J/mol&#xa0;K. Photocatalytic degradation under visible light (500&#xa0;µW/cm<sup>2</sup>) achieved 85.48% AO degradation within 120&#xa0;min, driven by reactive oxygen species (ROS) such as hydroxyl radicals (∙OH) and superoxide anions (O<sub>2</sub>∙⁻). The hybrid composite demonstrated excellent reusability, retaining 89.9% of its adsorption capacity after six cycles. These results highlight the CS-UiO-66-TiO<sub>2</sub> hybrid composite as a promising multifunctional material for sustainable wastewater purification.</p>

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Eco-Friendly Chitosan-UiO-66 MOF-TiO2 Hybrid Composite for the Efficient Adsorption and Photocatalytic Degradation of Carcinogenic Auramine O: A Sustainable Strategy for Wastewater Purification and Environmental Protection

  • Mohammad Hasan Al-Omari,
  • Saedah Rwede AL-Mhyawi,
  • Ahmed H. Ragab,
  • Ahmed Abu-Rayyan,
  • Mahmoud F. Mubarak,
  • Mohamed Hemdan

摘要

Developing advanced and eco-friendly materials for wastewater treatment is critical to addressing global water pollution. In this study, a novel chitosan–UiO-66 metal–organic framework (MOF)–TiO2 (CS-UiO-66-TiO2) hybrid composite was synthesized and evaluated for the removal of Auramine O (AO) via adsorption and photocatalysis. The hybrid composite exhibited a maximum adsorption capacity of 368.8 mg/g and a removal efficiency of 98.44% under optimal conditions (pH 6, 260 min, and 160 mg/L AO). Comprehensive characterization, including scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) surface area analysis, and thermogravimetric analysis (TGA), provided conclusive evidence that UiO-66 MOF and TiO2 were successfully integrated into the chitosan matrix, enhancing structural integrity and chemical reactivity. BET analysis revealed a high surface area of 786.84 m2/g, contributing to enhanced adsorption performance. The adsorption process was best described by the pseudo-second-order (PSO) kinetic model, demonstrating excellent agreement with experimental data in both linear (R2 = 0.998) and non-linear (R2 = 0.999) forms. Additionally, the Freundlich isotherm provided the best fit for the equilibrium data, with correlation coefficients of R2 = 0.999 (linear) and R2 = 0.998 (non-linear), indicating adsorption on a heterogeneous surface with multiple binding sites. Thermodynamic analysis confirmed the process was spontaneous and endothermic, with Gibbs free energy change (ΔG) ranging from − 5.43 to − 9.61 kJ/mol (298.15–338.15 K), enthalpy change (ΔH) of + 80.85 kJ/mol, and entropy change (ΔS) of + 37.85 J/mol K. Photocatalytic degradation under visible light (500 µW/cm2) achieved 85.48% AO degradation within 120 min, driven by reactive oxygen species (ROS) such as hydroxyl radicals (∙OH) and superoxide anions (O2∙⁻). The hybrid composite demonstrated excellent reusability, retaining 89.9% of its adsorption capacity after six cycles. These results highlight the CS-UiO-66-TiO2 hybrid composite as a promising multifunctional material for sustainable wastewater purification.