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Anion-adaptive crystalline cationic material for 99TcO4- trapping.

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.

SUBMITTER: Mei L

PROVIDER: S-EPMC6449352 | biostudies-literature | 2019 Apr

REPOSITORIES: biostudies-literature

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Anion-adaptive crystalline cationic material for 99TcO4- trapping.

Mei Lei L Li Fei-Ze FZ Li Fei-Ze FZ Lan Jian-Hui JH Wang Cong-Zhi CZ Xu Chao C Deng Hao H Wu Qun-Yan QY Hu Kong-Qiu KQ Wang Lin L Chai Zhi-Fang ZF Chen Jing J Gibson John K JK Shi Wei-Qun WQ

Nature communications 20190404 1

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 trap ...[more]

PMID: 30948745

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Project description:99Tc is one of the most problematic fission products in the nuclear fuel cycle owing to its large inventory in used nuclear fuel, long half-life, potential radiation hazard, high environmental mobility of its major species 99TcO4 -, and its redox-active nature. Ideally, 99TcO4 - should be removed at the first stage, when the used fuel rods are dissolved in highly concentrated nitric acid solution, which can substantially reduce its interference with the solvent extraction process through catalytic redox reactions with the key actinides and diminish the chance of discharge into the environment as the volatile species during the waste vitrification process. However, this task cannot be achieved by any of the reported anion-scavenging materials including traditional polymeric anion-exchange resins, inorganic cationic framework materials, and recently developed cationic metal-organic framework materials, because they either are not stable under the extreme conditions of the combined high acidity and strong radiation field or do not possess the required uptake selectivity towards 99TcO4 - in the presence of a huge excess of competing anions such as NO3 - and SO4 2-. Herein, we present the first study of 99TcO4 - removal under extreme conditions by a two-dimensional conjugated cationic covalent organic framework material, SCU-COF-1. This material exhibits ultrahigh acid stability, great resistance towards both large-dose β and γ irradiation and unprecedented 99TcO4 - uptake capabilities including extremely fast sorption kinetics (sorption equilibrium can be reached within 1 min), ultrahigh uptake capacity (702.4 mg g-1 for the surrogate ReO4 - at a slightly elevated temperature), and good anion-exchange selectivity towards 99TcO4 -. These excellent features endow SCU-COF-1 with the practical capabilities of separating 99TcO4 - from both simulant highly acidic fuel reprocessing solutions (3 M nitric acid) and low-activity waste streams at the US legacy nuclear site. The anion-exchange mechanism and the 99TcO4 - uptake selectivity are further demonstrated and clearly visualized by the molecular dynamics simulation investigations.

Dataset Information

Anion-adaptive crystalline cationic material for 99TcO4- trapping.

Publications

Anion-adaptive crystalline cationic material for <sup>99</sup>TcO<sub>4</sub><sup>-</sup> trapping.

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