"Ion-imprinting" strategy towards metal sulfide scavenger enables the highly selective capture of radiocesium.

Tang, Jun-Hao; Jia, Shao-Qing; Liu, Jia-Ting; Yang, Lu; Sun, Hai-Yan; Feng, Mei-Ling; Huang, Xiao-Ying · Nat Commun · 2024

basic_science · Level V

Where this comes from

Abstract

Highly selective capture of radiocesium is an urgent need for environmental radioactive contamination remediation and spent fuel disposal. Herein, a strategy is proposed for construction of "inorganic ion-imprinted adsorbents" with ion recognition-separation capabilities, and a metal sulfide Cs<sub>2.33</sub>Ga<sub>2.33</sub>Sn<sub>1.67</sub>S<sub>8</sub>·H<sub>2</sub>O (FJSM-CGTS) with "imprinting effect" on Cs<sup>+</sup> is prepared. We show that the K<sup>+</sup> activation product of FJSM-CGTS, Cs<sub>0.51</sub>K<sub>1.82</sub>Ga<sub>2.33</sub>Sn<sub>1.67</sub>S<sub>8</sub>·H<sub>2</sub>O (FJMS-KCGTS), can reach adsorption equilibrium for Cs<sup>+</sup> within 5 min, with a maximum adsorption capacity of 246.65 mg·g<sup>-1</sup>. FJMS-KCGTS overcomes the hindrance of Cs<sup>+</sup> adsorption by competing ions and realizes highly selective capture of Cs<sup>+</sup> in complex environments. It shows successful cleanup for actual <sup>137</sup>Cs-liquid-wastes generated during industrial production with removal rates of over 99%. Ion-exchange column filled with FJMS-KCGTS can efficiently treat 540 mL Cs<sup>+</sup>-containing solutions (31.995 mg·L<sup>-1</sup>) and generates only 0.12 mL of solid waste, which enables waste solution volume reduction. Single-crystal structural analysis and density functional theory calculations are used to visualize the "ion-imprinting" process and confirm that the "imprinting effect" originates from the spatially confined effect of the framework. This work clearly reveals radiocesium capture mechanism and structure-function relationships that could inspire the development of efficient inorganic adsorbents for selective recognition and separation of key radionuclides.