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Efficient and selective extraction of uranium (U(VI)) from seawater is essential for sustainable nuclear power production. This study reports a novel adsorbent zeolitic imidazolate framework (ZIF)-67@SiO2-A/polyacrylamide (PAM) which was synthesized by grafting the core–shell metal–organic frameworks (MOFs)-based nanostructures coated with the 3-aminopropyl triethoxysilane (APTES) functionalized SiO2 (SiO2-A) onto PAM hydrogel. The SiO2 shell was grown on the surface of MOF, which improved the acid-base resistance of MOF. The introduction of ZIF-67@SiO2-A enhances the specific surface area and adsorption efficiency of the PAM. The ZIF-67@SiO2-A/PAM shows remarkable adsorption capacity, fast adsorption kinetics, and good reusability for uranium. It has excellent adsorption property (6.33 mg·g−1, 30 d) in natural seawater. The X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR), energy dispersive spectroscopy (EDS) mappings, and density functional theory reveal that the coordination by N and O in ZIF-67@SiO2-A/PAM with uranium is the main mechanism of uranium adsorption. Thus, ZIF-67@SiO2-A/PAM has great potential to capture uranium from natural seawater.

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