Dataset Information

Optimizing Strategy for Enhancing the Stability and ⁹⁹TcO₄ ^- Sequestration of Poly(ionic liquids)@MOFs Composites.

ABSTRACT: Metal-organic frameworks (MOFs) are a class of promising sorbents for effective sequestration of radioactive ⁹⁹TcO₄ ^- anions. However, their poor stability and slow sorption kinetics in the industrial condition pose a great challenge. Herein, we demonstrate an optimizing strategy via in situ polymerization of ionic liquids (ILs) encapsulated in the pores of MOFs, forming polyILs@MOFs composites with greatly enhanced TcO₄ ^- sequestration compared with the pristine MOFs. Notably, the cross-linked polymerization of ILs facilitates the formation of both the inside ionic filler as the active sites and outside coating as the protective layers of MOFs, which is significantly beneficial to obtain the optimized sorption materials of exceptional stability under extreme conditions (e.g., in 6 M HNO₃). The final optimized composite shows fast sorption kinetics (<30 s), good regeneration (>30 cycles), and superior uptake performance for TcO₄ ^- in highly acidic conditions and simulated recycle stream. This strategy opens up a new opportunity to construct the highly stable MOF-based composites and extend their applicability in different fields.

SUBMITTER: Li CP

PROVIDER: S-EPMC7760461 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Optimizing Strategy for Enhancing the Stability and 99TcO4 - Sequestration of Poly(ionic liquids)@MOFs Composites.

Li Cheng-Peng CP Li Hai-Ruo HR Ai Jin-Yun JY Chen Jing J Du Miao M

ACS central science 20201130 12

Metal-organic frameworks (MOFs) are a class of promising sorbents for effective sequestration of radioactive 99TcO4 - anions. However, their poor stability and slow sorption kinetics in the industrial condition pose a great challenge. Herein, we demonstrate an optimizing strategy via in situ polymerization of ionic liquids (ILs) encapsulated in the pores of MOFs, forming polyILs@MOFs composites with greatly enhanced TcO4 - sequestrati ...[more]

PMID: 33376797

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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

Optimizing Strategy for Enhancing the Stability and ⁹⁹TcO₄ ^- Sequestration of Poly(ionic liquids)@MOFs Composites.

Publications

Optimizing Strategy for Enhancing the Stability and <sup>99</sup>TcO<sub>4</sub> <sup>-</sup> Sequestration of Poly(ionic liquids)@MOFs Composites.

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