Kinetics, Isotherm, Mechanism, and Recyclability of Novel Nano-sized Ce4+-Doped Ni-Al Layered Double Hydroxide for Defluoridation of Aqueous Solutions

Abstract

Abstract Excessive fluoride removing from aqueous solutions is of utmost importance as it has adverse impact on human health. This study investigates the defluoridation efficiency of a novel nano-sized Ce+4-doped Ni/Al layered double hydroxide (Ni-Al-Ce LDH) for aqueous solutions. The synthesized Ni-Al-Ce LDH exhibited a well-defined nanoscale plate-like morphology and a high surface area with an average size of 11.51 nm, which contributed to its enhanced fluoride adsorption capacity. XRD, SEM, HRTEM, and BET studies confirmed these characteristics. XPS analysis confirmed the presence of Ce4+ ions within the Ni-Al LDH. The experimental results indicated that the process of defluoridation followed a pseudo-second order model of kinetics, suggesting a chemisorption mechanism. The fluoride adsorption isotherms demonstrated well fits to the Freundlich, Langmuir and Jovanovic models, indicating both monolayer and multilayer fluoride adsorption on the Ce-doped Ni-Al LDH. The maximum adsorption capacity was found to be 238.27 mg/g (Langmuir) and 130.73 mg/g (Jovanovic) at pH 6.0 and 25°C. The proposed mechanisms for fluoride adsorption on the LDH include ion exchange, surface complexation, hydrogen bonding, and ligand exchange. The Ni-Al-Ce LDH nanomaterial exhibited good recyclability, maintaining 71% of the fluoride adsorption efficiency even after four consecutive cycles. This study highlights the significant role of Ce doping in improving the performance of Ni-Al LDH as a defluoridation adsorbent.