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Removal of uranium from radioactive wastewater with TPEAC. [Display omitted] • A phosphine-oxime modified adsorbent (TPEAC) was successfully prepared. • TPEAC exhibited exceptional selectivity and efficiency for adsorption of uranium. • TPEAC displayed a high recovery of 99.6% using real uranium mining wastewater. • Adsorption mechanism was elucidated through experiments and characterization. Efficient removal of uranium from radioactive wastewater is paramount for the sustainable development of nuclear energy. However, the exploitation of superior adsorbents with practical applications remains a challenge. In this work, we engineered and synthesized an adsorbent (TPEAC) enriched with phosphine-oxime, featuring a matrix composed of hydrophilic modified amidoxime functional groups. TPEAC exhibited exceptional selectivity (Multiple ion coexistence R% > 99 %) and efficiency in uranium adsorption, with a higher adsorption rate (reach equilibrium around 400 mins) and capacity (243.9 mg/g) than raw-amidoxime (133.3 mg/g) and modified-amidoxime (175.4 mg/g) materials. Moreover, it maintained robust stability and reusability even after six adsorption–desorption cycles, with removal ratio still above 95 %. In-depth mechanistic investigations through DFT and XPS elucidated that P-O (P=O) groups exhibited a stronger affinity for U(VI) compared to other functional groups, and the adsorption of TPEAC towards U(VI) primarily due to the synergistic interaction among P-O (P=O) groups, C(NH 2) = N-OH, and carboxyl groups, which significantly facilitated the effective removal of U(VI). Most prominently, TPEAC performed considerable potential in processing actual uranium mine wastewater, with its dynamic column device achieving a U(VI) recovery up to 99.6 %. This work not only furnishes an efficacious and economical solution for uranium wastewater treatment but also provides new approaches for scalable application uranium materials. [ABSTRACT FROM AUTHOR]

• A highly efficient adsorbent was prepared and used for the treatment of uranium wastewater. • MXene/PAO hydrogel beads exhibit outstanding adsorption capacity under different conditions. • MXene/PAO hydrogel beads have excellent practicality coupling through columns. • Adsorption mechanism under F− conditions is the coordination of MXene and amidoxime to uranium complexes. The treatment of radioactive wastewater is crucial to ensure the safe and rapid development of nuclear energy. However, efficient disposal of uranium wastewater containing high concentrations of fluoride ions (F−) generated during uranium enrichment and conversion poses a formidable and pressing challenge. In this study, we successfully synthesized MXene/PAO hydrogel beads (MPH beads) by self-assembling two-dimensional Ti 3 C 2 T x MXene nanosheets with amidoxime through ionic cross-linking. MPH beads exhibited exceptional uranium adsorption capacity (625 mg/g), remarkable adsorption selectivity, and good reusability. Notably, MPH beads demonstrated a maximum uranium adsorption capacity of 400 mg/g in an aqueous solution containing 8000 ppm F−. Furthermore, MPH beads showed favorable F− resistance and were able to remove>95% of U(Ⅵ) even after being immersed in an extreme environment for 15 days. Additionally, MPH beads achieved a high U(Ⅵ) recovery of 98.2% from real environment water samples using dynamic column experiments, showcasing their excellent application performance. The efficient U(Ⅵ) adsorption and anti-fluoride effect were mainly attributed to the combined complexation between the C(NH 2) = N-OH, C-Ti-OH groups and U(Ⅵ), as demonstrated by experiments, characterization, and DFT calculations. Our study highlights the significant potential of MPH beads in the treatment of uranium from radioactive wastewater, especially wastewater with high concentrations of F−. [ABSTRACT FROM AUTHOR]