The uranium level in seawater is ≈1000 times as high as terrestrial ores and can provide potential near‐infinite fuel for the nuclear energy industry. However, it is still a significant challenge to develop high‐efficiency and low‐cost adsorbents for massively extracting uranium from seawater. Herein, a simple and fast method through low‐energy consumption sunlight polymerization to direct fabrication of a poly(amidoxime) (PAO) hydrogel membrane, which exhibits high uranium adsorption capacity, is reported. This PAO hydrogel owns semi‐interpenetrating structure and a hydrophilic poly(acrylamide) 3D network of hydrogel which can disperse and fix PAOs well. As a result, the amidoxime groups of PAOs exhibit an outstanding uranium adsorption efficiency (718 ± 16.6 and 1279 ± 14.5 mg g −1 of m uranium / m PAO in 8 and 32 ppm uranium‐spiked seawater, respectively) among reported hydrogel‐based adsorbents. Most importantly, U‐uptake capacity of this hydrogel can achieve 4.87 ± 0.38 mg g −1 of m uranium / m dry gel just after four weeks within natural seawater. Furthermore, this hydrogel can be massively produced through low‐energy consumption and environmentally‐friendly sunlight polymerization. This work will provide a high‐efficiency and low‐cost adsorbent for massive uranium extraction from seawater.

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Uranium is an extremely abundant resource in seawater that could supply nuclear fuel for over the long-term, but it is tremendously difficult to extract. Here, a new supramolecular poly­(amidoxime) (PAO)-loaded macroporous resin (PLMR) adsorbent has been explored for highly efficient uranium adsorption. Through simply immersing the macroporous resin in the PAO solution, PAOs can be firmly loaded on the surface of the nanopores mainly by hydrophobic interaction, to achieve the as-prepared PLMR. Unlike existing amidoxime-based adsorbents containing many inner minimally effective PAOs, almost all the PAOs of PLMR have high uranium adsorption efficiency because they can form a PAO-layer on the nanopores with molecular-level thickness and ultrahigh specific surface area. As a result, this PLMR has highly efficient uranium adsorbing performance. The uranium adsorption capacity of the PLMR was 157 mg/g (the U PAO in the PLMR was 1039 mg/g), in 32 ppm uranium-spiked seawater for 120 h. Additionally, uranium in 1.0 L 100 ppb U-spiked both water and seawater can be removed quickly and the recovery efficiency can reach 91.1 ± 1.7% and 86.5 ± 1.9%, respectively, after being filtered by a column filled with 200 mg PLMR at 300 mL/min for 24 h. More importantly, after filtering 200 T natural seawater with 200 g PLMR for only 10 days, the uranium-uptake amount of the PLMR reached 2.14 ± 0.21 mg/g, and its average uranium adsorption speed reached 0.214 mg/(g·day) which is very fast among reported amidoxime-based adsorbents. This new adsorbent has great potential to quickly and massively recover uranium from seawater and uranium-containing wastewater. Most importantly, this work will provide a simple but general strategy to greatly enhance the uranium adsorption efficiency of amidoxime-functionalized adsorbents with ultrahigh specific surface area via supramolecular interaction, and even inspire the exploration of other adsorbents.

Although metal–organic frameworks (MOFs) own excellent uranium adsorption capacity but are still difficult to conveniently extract uranium from seawater due to the discrete powder state. In this study, a new MOF-based macroporous membrane has been explored, which can high-efficiently extract uranium through continuously filtering seawater. Through modifying the UiO-66 with poly(amidoxime) (PAO), it can disperse well in a N,N-dimethylformamide solution of graphene oxide and cotton fibers. Then, the as-prepared super-hydrophilic MOF-based macroporous membrane can be fabricated after simple suction filtration. Compared with nonmodified MOFs, this UiO-66@PAO can be dispersed uniformly in the membrane because it can stabilize well in the solution, which have largely enhanced uranium adsorbing capacity owing to the modified PAO. Last but not least, different from powder MOFs, this UiO-66@PAO membrane provides the convenient and continuously uranium adsorbing process. As a consequence, the uranium extraction capacity of this membrane can reach 579 mg·g−1 in 32 ppm U-added simulated seawater for only 24 h. Most importantly, this UiO-66@PAO membrane (100 mg) can remove 80.6% uranyl ions from 5 L seawater after 50 filtering cycles. This study provides a universal method to design and fabricate a new MOF-based adsorbent for high-efficient uranium recovery from seawater.

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