New materials based on clays modified with peptide complexes were synthesized for the first time for the removal of azo dyes using Advanced Oxidation Processes (AOP). The synthesis strategy involves silanization with APTES, covalent grafting of a peptide spacer (triglycine) via EDC/NHS activation, and final chelation of metal cations (Fe3⁺, Co ⁺, Ni ⁺, Cu ⁺). The synthesis steps were confirmed using various characterization techniques, namely N₂ adsorption-desorption, XRD, FTIR, SEM-EDX, SAA, ATG-ATD, and acidity measurements. These hybrid materials have been successfully applied to the degradation of Congo Red using various Advanced Oxidation Processes (AOPs): Fenton, photocatalysis (UV), and photo-Fenton. Finally, the impact of operating parameters (pH, catalyst mass, time, and H₂O₂ dose) was rigorously optimized using a full factorial design (2⁴ = 16 experiments), ensuring maximum decolorization efficiency of up to 97%.
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