Valorization of Phosphate Tailings into Ca-Mg-Al Layered Double Hydroxides for Phosphate Adsorption from Wastewater

Phosphate tailings (PTs), a solid waste generated from phosphate flotation, are a low-grade phosphate resource rich in quartz and dolomite. Their long-term accumulation leads to both resource loss and environmental risks, making valorization increasingly important for the sustainable development of the phosphorus chemical industry. In this study, calcareous–magnesian PTs were used as raw materials, and selective hydrothermal leaching with weakly acidic AlCl₃ solution was employed to separate the dolomite phase and directly construct a Ca-Mg-Al precursor solution for layered double hydroxides (LDHs). The LDHs were subsequently synthesized by co-precipitation and evaluated for phosphate removal from wastewater. The results showed that the precipitation pH markedly affected the phase composition and platelet morphology of the LDHs, while appropriate aging conditions further improved their adsorption performance. Under the optimal conditions of pH 12, aging at 40 °C for 2 h, the obtained LDHs exhibited the best phosphate uptake. Adsorption kinetics followed the pseudo-second-order model, and the maximum adsorption capacity calculated from the Langmuir model reached 38.61 mg-P/g. Characterization by XRD, FTIR, TG-DTA, point of zero charge, and XPS indicated that phosphate removal was dominated by surface complexation, accompanied by anion exchange, ionic precipitation, and electrostatic attraction.