Abstract
Efficient anion recognition is of great significance for radioactive 99TcO4− decontamination, but it remains a challenge for traditional sorbents. Herein, we put forward a tactic using soft crystalline cationic material with anion-adaptive dynamics for 99TcO4− sequestration. A cucurbit[8]uril-based supramolecular metal-organic material is produced through a multi-component assembly strategy and used as a sorbent for effective trapping of TcO4−. Excellent separation of TcO4−/ReO4− is demonstrated by fast removal kinetics, good sorption capacity and high distribution coefficient. Remarkably, the most superior selectivity among metal-organic materials reported so far, together with good hydrolytic stability, indicates potential for efficient TcO4− removal. The structure incorporating ReO4− reveals that the supramolecular framework undergoes adaptive reconstruction facilitating the effective accommodation of TcO4−/ReO4−. The results highlight opportunities for development of soft anion-adaptive sorbents for highly selective anion decontamination.
Highlights
Efficient anion recognition is of great significance for radioactive 99TcO4− decontamination, but it remains a challenge for traditional sorbents
The nitrate counterions are located in tetrahedral cavities formed by four neighboring CB8 from the 1D chains (Fig. 2d, e and Supplementary Figure 9), and contributed a lot to the formation of final supramolecular framework via anion-directed assembly (Fig. 2f)
Besides the Electrostatic potential (ESP) maps, hydrogen bonding orbital interaction analysis from the MO perspective were studied, and the results reveal that orbital interactions contribute to several hydrogen bonds as evidenced by that of [H] and ReO4− (Supplementary Figure 27)
Summary
Efficient anion recognition is of great significance for radioactive 99TcO4− decontamination, but it remains a challenge for traditional sorbents. Excellent separation of TcO4−/ReO4− is demonstrated by fast removal kinetics, good sorption capacity and high distribution coefficient. The most superior selectivity among metal-organic materials reported so far, together with good hydrolytic stability, indicates potential for efficient TcO4− removal. Solvent extraction and ion exchange are two well-established effective methods for removal of TcO4− from aqueous media[3,4,5,6]. Despite the ease of implementation and the expected efficient recovery of TcO4− based on ion-exchange method[5,10], the total performance of sorbent materials used seems not to be competent. There is still demand for improvement in terms of selectivity of TcO4− sorbents, with enhanced discrimination for TcO4−/ReO4− over other anions as a desirable attribute
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