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The extremely high adsorption efficiency of malachite green (MG) was examined through a series of batch experiments by using Fe 3+ -doped Mg/Al layered double hydroxides (LDHs). The incorporation of iron into Mg/Al LDH with varying Al + Fe molar ratio of 4 + 1, 3 + 2, 2 + 3, and 1 + 4 increased the adsorption capacity with respect to time. The spectral analysis and N 2 sorption studies showed that there was retention of surface morphology in all of the iron-modified LDH samples. The experimental evidences showed that the adsorbent Mg/(Al + Fe) with a molar ratio of 10:2 + 3 had a significant removal, i.e., 99.94% for MG with the initial concentration of 1000 mg L –1 at pH ∼ 9 and at room temperature in 5 min. With further increase in iron loading (at ratio 10:1 + 4), there was a decrease in the removal of MG due to the agglomeration of Fe 2 O 3 on the surface. The adsorption process was best fitted to the Freundlich isotherm followed by the pseudo-second-order model. The standard thermodynamic parameters (Δ H °, Δ S °, and Δ G °) were obtained over the temperature range of 20–50 °C. It was observed that the adsorption of MG onto Mg/(Al + Fe) LDH was spontaneous, exothermic, and enthalpy driven in the physisorption mode. A worthy desorption efficiency was achieved by using ethanol and water, which was more than 90% in the three cycles. Maintaining almost the same removal efficiency of MG even after three cycles indicated Mg/(Al + Fe) LDH as a promising material for wastewater treatment. This work was anticipated to open up new possibilities in dealing with anionic dye pollutants.

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