In-situ growth of hierarchical layered double hydroxide on polydopamine-encapsulated hollow Fe₃O₄ microspheres for efficient removal and recovery of U(VI)

With the increasing demand of nuclear power plant, the depleted uranium is inevitably emitted and causes environmental risk, hence it is crucial to develop new methods to efficiently eliminate uranium compounds from water. In this work, a bifunctional material core-shell-shell layered double hydroxide (LDH) decorated hollow magnetic polydopamine (MP) microspheres (defined as MPL) were synthesized and evaluated for the cleanup of uranium (VI) from aqueous solutions through specific adsorption. The experimental results showed that the adsorption was significantly affected by pH value rather than ionic strength, reflecting that the interaction was mainly governed by inner-sphere surface complexation owing to the multiple functional groups including imine, catechol, amine, and hydroxyl groups. The adsorption kinetics can be perfectly depicted by the pseudo-second-order model with high uptake percentage of 94.8%, which was superior to the previously reported materials. Interestingly, the maximum adsorption performance can be tuned by changing the thickness of polydopamine shell and the content of LDH, in the order of MP₂L₂ (344 mg/g) > MP₂L₃ (291 mg/g) > MP₃L₂ (245 mg/g) > MP₂L₁ (211 mg/g) > ML₂ (142 mg/g) > MP₁L₂ (141 mg/g) > MP₂ (71 mg/g) > Fe₃O₄ (34 mg/g) at 298.15 K and pH 5.0. The adsorption mechanism has been thoroughly investigated with techniques such as transmission electron microscopy (TEM), scanning electron microscopy (SEM), vibrating sample magnetometer (VSM), X-ray diffraction (XRD), thermo-gravimetric analyses (TGA), Fourier transformed infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). In summary, the bifunctional material could be applied as promising building block for the enrichment and recovery of uranium (VI) from aqueous solutions in environmental pollution cleanup.