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An ionic vinylene-linked three-dimensional covalent organic framework for selective and efficient trapping of ReO₄^- or ⁹⁹TcO₄.

ABSTRACT: The synthesis of ionic olefin linked three-dimensional covalent organic frameworks (3D COFs) is greatly challenging given the hardness of the formation of stable carbon-carbon double bonds (-C = C-). Herein, we report a general strategy for designing porous positively charged sp² carbon-linked 3D COFs through the Aldol condensation promoted by quaternization. The obtained 3D COFs, namely TFPM-PZI and TAPM-PZI, showed impressive chemical stability. Furthermore, the positively charged frameworks with regular porosity endow 3D ionic COFs with selective capture radioactive ReO₄^-/TcO₄^- and great removal efficiency in simulated Hanford waste. This research not only broadens the category of 3D COFs but also promotes the application of COFs as efficient functional materials.

SUBMITTER: Zhang CR

PROVIDER: S-EPMC9734744 | biostudies-literature | 2022 Dec

REPOSITORIES: biostudies-literature

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An ionic vinylene-linked three-dimensional covalent organic framework for selective and efficient trapping of ReO4- or 99TcO4.

Zhang Cheng-Rong CR Cui Wei-Rong WR Yi Shun-Mo SM Niu Cheng-Peng CP Liang Ru-Ping RP Qi Jia-Xin JX Chen Xiao-Juan XJ Jiang Wei W Liu Xin X Luo Qiu-Xia QX Qiu Jian-Ding JD

Nature communications 20221209 1

The synthesis of ionic olefin linked three-dimensional covalent organic frameworks (3D COFs) is greatly challenging given the hardness of the formation of stable carbon-carbon double bonds (-C = C-). Herein, we report a general strategy for designing porous positively charged sp2 carbon-linked 3D COFs through the Aldol condensation promoted by quaternization. The obtained 3D COFs, namely TFPM-PZI and TAPM-PZI, showed impressive chemical stability. Furthermore, the positively charged f ...[more]

PMID: 36494388

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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

An ionic vinylene-linked three-dimensional covalent organic framework for selective and efficient trapping of ReO₄^- or ⁹⁹TcO₄.

Publications

An ionic vinylene-linked three-dimensional covalent organic framework for selective and efficient trapping of ReO<sub>4</sub><sup>-</sup> or <sup>99</sup>TcO<sub>4</sub>.

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