Controllable Synthesis of Ca-Mg-Al Layered Double Hydroxides and Calcined Layered Double Oxides for the Efficient Removal of U(VI) from Wastewater Solutions

Novel rod-like ternary nanoscale layered double hydroxides (Ca-Mg-Al-LDH) and their bimetal derivatives (Ca-Mg-Al-LDOx, x: 200, 300, 400, 500, and 600 °C) were fabricated with a simple-green hydrothermal and calicination process. The interaction mechanism and adsorption property of U(VI) on Ca-Mg-Al-LDH and Ca-Mg-Al-LDOx were investigated by a batch technique and spectroscopy analysis, and the results indicated that U(VI) could form strong and stable surface complexes on Ca-Mg-Al-LDH and Ca-Mg-Al-LDOx surfaces. The adsorption capacity of U(VI) on various adsorbents could be controlled and adjusted through changing the calcination temperature, which was attributed to the different contents of various metal-oxide bonds (e.g., Ca-O, Mg-O, and Al-O). The adsorption capacities of U(VI) on these adsorbents were in the order of Ca-Mg-Al-LDO500 (486.8 mg/g) > Ca-Mg-Al-LDO600 (373.4 mg/g) > Ca-Mg-Al-LDO400 (292.5 mg/g) > Ca-Mg-Al-LDO300 (260.0 mg/g) > Ca-Mg-Al-LDO200 (223.5 mg/g) > Ca-Mg-Al-LDH (132.5 mg/g), which might be attributed to more active surface sites and abundant "Ca-O and Al-O" with the increase of calcination temperature. The results of kinetic and thermodynamic studies demonstrated that the adsorption was a spontaneous and endothermic chemical process, and the better fitted Sips model revealed that the adsorption reaction was multilayer adsorption at low concentration of U(VI) and monolayer adsorption at high concentration of U(VI). This study provided highlights on the interaction mechanism of U(VI) with various metal-oxide bonds, and it could play an important role for the controllable adsorption capacity and effcient application in environmental remediation.