Eco-Friendly Orange Peels/Aluminum/Graphene Oxide Composites for Reactive Red 120 and Methylene Violet Dye Removal from Textile Wastewater

In this work, sustainable aluminum-modified orange peels functionalized with graphene oxide (OP-Al-GO) were synthesized and evaluated for the removal of Methylene Violet (MV) and Reactive Red 120 (RR120) from aqueous solutions. Adsorption performance was systematically investigated in single-dye systems, binary dye mixtures, and real textile wastewater samples, and compared with that of orange peels (OP), orange peel–aluminum composite (OP-Al), and graphene oxide (GO). pHpzc analysis clarified the surface charge of the adsorbent, while SEM and FTIR showed that the incorporation of aluminum and GO increased roughness and functional groups appearance, enhancing dye adsorption and confirming successful interactions. The OP-Al-GO composites exhibited improved removal efficiency for both dyes (64.8% for RR120 and 96.2% for MV) at pH 3.0. The presence of aluminum improved structural stability and surface charge regulation, while graphene oxide contributed to multiple adsorption mechanisms, including electrostatic attraction and π–π interactions. The adsorption kinetics were found to follow a pseudo-second-order (PSO) kinetic model for RR120 and an intraparticle-diffusion model (IPD) for MV, while isotherm analysis revealed a Langmuir behavior for MV and a Freundlich behavior for RR120. Langmuir maximum adsorption capacities were 298.7 and 10.8 mg/g for MV and RR120, respectively. High removal efficiency was maintained in binary dye mixtures, with OP-Al-GO achieving 96.9% removal of MV and 85.7% of RR120. Furthermore, the proposed adsorbent was tested on real wastewater samples, and the results highlight that the proposed adsorbents are promising, low-cost, and environmentally sustainable for textile wastewater treatment.