Enhancing adsorptive performance of Cu-Al layered double hydroxides from aluminum saline slags: Insights from response surface methodology and molecular dynamic simulation

Abstract

This study aims to optimize the adsorption process of gallic acid (GA) on Cu-Al layered double hydroxides (LDHs) synthesized via a co-precipitation method at various pH levels. The procedure is based on the adsorption of organic pollutants from aqueous solutions, with evaluations carried out based on operational parameters such as pH, initial concentration, and adsorbent quantity. Two series of LDHs were compared: one using aluminum extracted from saline slags and the other using a commercial aluminum salt as source of aluminum. Saline slags, a by-product of aluminum recycling, are particularly hazardous due to their high toxicity and potential for environmental contamination. Extracting aluminum from these slags and using it in the synthesis of LDHs not only helps in eliminating a dangerous waste but also creates materials with beneficial environmental applications. The adsorption process was optimized using response surface methodology (RSM) coupled with Box-Behnken design (BBD) to assess the effects of key operational parameters. Besides gallic acid, other organic pollutants such as diclofenac and salicylic acid were also evaluated for removal from aqueous solution. The LDH /LDO were characterized by X-ray diffraction (XRD), ATR infrared spectroscopy (ATR-IR), scanning and transmission electron microscopy (SEM/TEM), thermogravimetric analysis (TGA), and nitrogen adsorption at −196 °C. The merit data indicate that the material synthesized at pH = 9 with extracted aluminum exhibits superior adsorption capacity for gallic acid, demonstrating the highest removal rate, nearly reaching 100 %, and achieving equilibrium more quickly than other samples. This superior adsorption performance is also notable for salicylic acid and diclofenac. After four regeneration cycles, the adsorption rate of the adsorbent remains stable, indicating that CCA9 maintains a consistent and efficient adsorption performance. This highlights the robustness of the material and its high reusability in prolonged adsorption applications. Molecular dynamics simulations (MDS) revealed that the adsorption process occurs spontaneously, driven by weak interactions: van der Waals, intermolecular, hydrogen bonding, π-interactions and short contacts.