Green magnetite/carbonized spent coffee (MG/CFC) composite was synthesized from natural pyrite and characterized as an adsorbent and catalyst in photo-Fenton’s oxidation system of Congo red dye (C.R). The absorption behavior was illustrated based on the steric and energetic parameters of the advanced Monolayer equilibrium model of one energetic site (R2 > 0.99). The structure exhibits 855 mg/g as effective site density which induces its C.R saturation adsorption capacity to 436.1 mg/g. The change in the number of absorbed C.R per site with temperature (n = 1.53 (293) to 0.51 (313 K)) suggests changes in the mechanism from multimolecular (up to 2 molecules per site) to multianchorage (one molecule per more than one site) processes. The energetic studies (ΔE = 6.2–8.2 kJ/mol) validate the physical uptake of C.R by MG/CFC which might be included van der Waals forces, electrostatic attractions, and hydrogen bonding. As a catalyst, MG/CFC exhibits significant activity during the photo-Fenton’s oxidation of C.R under visible light. The complete oxidation of C.R was detected after 105 min (5 mg/L), 120 min (10 mg/L), 135 min (15 mg/L), 180 min (20 mg/L), and 240 min (25 mg/L) using MG/CFC at 0.2 g/L dosage and 0.1 mL of H2O2. Increasing the dosage up to 0.5 g/L reduce the complete oxidation interval of C.R (5 mg/L) down to 30 min while the complete mineralization was detected after 120 min. The acute and chronic toxicities of the treated samples demonstrate significant safe products of no toxic effects on aquatic organisms as compared to the parent C.R solution.
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