Adsorption of the hazardous dye malachite green (MG) by Acacia nilotica (AN) waste was investigated. Batch process variables for the adsorption of MG by AN were optimized. The mechanisms involved in the adsorption of MG by AN were explored using isotherms and kinetic models. The thermodynamic parameters were calculated to determine the spontaneity and thermal nature of the MG adsorption reaction. The maximum equilibrium adsorption capacity of AN was found to be 113.26 mg/g at 30 °C. The MG adsorption data revealed that AN adsorbs MG by multilayer adsorption, as shown by the better fit of the data to the Freundlich and Halsey models (R2 = 0.99) rather than to the Langmuir model. Multilayer adsorption involves physisorption, which was confirmed by the E value (mean free energy of adsorption) of the Dubinin–Radushkevich model (6.52 kJ/mol). Surface diffusion was found to be the main driving force for MG adsorption by AN. The MG adsorption reaction was endothermic, based on the enthalpy, and was controlled by the entropy of the system in the T1 temperature range (30 to 40 °C), while the opposite trend was observed in the T2 range (40 to 50 °C). Moreover, MG adsorption by AN was found to be nonspontaneous at all temperatures.

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