“Ion-imprinting” strategy towards metal sulfide scavenger enables the highly selective capture of radiocesium

• Published in: Nature communications Vol. 15; no. 1; p. 4281
• Main Authors: Tang, Jun-Hao, Jia, Shao-Qing, Liu, Jia-Ting, Yang, Lu, Sun, Hai-Yan, Feng, Mei-Ling, Huang, Xiao-Ying
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 20-05-2024; Nature Publishing Group; Nature Portfolio
• Subjects: 140/146; 639/638/169; 639/638/263; 639/638/298; 639/638/903; Adsorbents; Adsorption; Cesium 137; Cesium isotopes; Cesium radioisotopes; Density functional theory; Environmental cleanup; Humanities and Social Sciences; Industrial production; Ion exchange; multidisciplinary; Radioactive contamination; Radioactive pollution; Radioisotopes; Recognition; Remediation; Science; Science (multidisciplinary); Separation; Single crystals; Solid wastes; Spent nuclear fuels; Structural analysis; Structure-function relationships; Sulfides
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-48565-x

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
2.33
Ga
2.33
Sn
1.67
S
8
·H
2
O (FJSM-CGTS) with “imprinting effect” on Cs
+
is prepared. We show that the K
+
activation product of FJSM-CGTS, Cs
0.51
K
1.82
Ga
2.33
Sn
1.67
S
8
·H
2
O (FJMS-KCGTS), can reach adsorption equilibrium for Cs
+
within 5 min, with a maximum adsorption capacity of 246.65 mg·g
−1
. FJMS-KCGTS overcomes the hindrance of Cs
+
adsorption by competing ions and realizes highly selective capture of Cs
+
in complex environments. It shows successful cleanup for actual
137
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
+
-containing solutions (31.995 mg·L
−1
) 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.
Selective capture of radiocaesium is highly challenging in radioactive contamination remediation. Here, authors developed “ion-imprinting” strategy towards metal sulfide scavengers to achieve selective capture of Cs(I) in high-salt environments and successful cleanup of actual 137Cs-liquid-wastes.