This work utilized a one-pot synthesis method to synthesize Cu/Fe/Al mixed metal oxide (MMO) from layered double hydroxide (LDH) calcination. The adsorption potentials of Cu/Fe/Al LDH and Cu/Fe/Al MMOs were evaluated using Congo Red (CR) aqueous solution. Various advanced techniques were used to characterize the synthesized nanomaterial. XRD confirmed the successful synthesis of trimetallic carbonate intercalated LDH and MMO, while FE-SEM revealed their flaky morphology. EDX and FT-IR analyses supported the dye removal mechanism, showing that MMOs had greater adsorptive removal of CR molecules than LDH. This was primarily due to the MMOs' larger surface area and microporous structure (132 m²/g) which favoured greater adsorption. The adsorption kinetics reveal that the adsorptive removal of CR on LDH and MMOs follows a pseudo-second-order reaction. Moreover, as predicted by Freundlich the maximum adsorptive removal was obtained by LDH-derived MMO (96%) which was higher than the LDH (90%). The thermodynamics indicates that adsorption was exothermic and thus more favorable at room temperature. In addition, the Box-Behnken Design (BBD) was adopted for Response Surface Methodology (RSM) due to its simplicity in analysis and effectiveness in systematically evaluating the impact of pH, dosage of adsorbent, dye concentration, contact period, and temperature variables. The pHzpc of 7.9 indicated that lower pH enhances adsorption, and a +5.1 mV charge on the MMO surface, measured by zeta potential, supported electrostatic interaction with the anionic dye. Lastly, LDH and LDH-derived MMO were regenerated using 1 M NaOH and effectively reused for up to 5 cycles. MMOs demonstrated superior reusability compared to LDH for anionic dye removal. Thus, the synthesised Cu/Fe/Al MMO, with its large surface area, offers a superior adsorbent for removing organic pollutants.
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