Journal
DALTON TRANSACTIONS
Volume 51, Issue 42, Pages 16170-16180Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2dt02371g
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Funding
- French State under the program Investissements d'Avenir [ANR-11-RSNR-0013-01]
- Chevreul Institute [FR 2638]
- Ministere de l'Enseignement Superieur et de la Recherche
- Region Hauts de France
- FEDER
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This study reports the capture and immobilization of gaseous RuO4 using a porous metal-organic framework (UiO-66-NH2) for the first time. UiO-66-NH2 exhibits remarkable affinity for RuO4 capture, resulting in the highest RuO4 decontamination factor worldwide. The efficiency of UiO-66-NH2 can be attributed to its pore diameters well adapted for RuO4 capture and its conversion into stable RuO2.
Ru-106 is a radioactive isotope usually generated by the nuclear industry within power plant reactors. During a nuclear accident, Ru-106 reacts with oxygen, leading to the production of highly volatile ruthenium tetroxide RuO4. The combination of volatility and radioactivity makes (RuO4)-Ru-106, one of the most radiotoxic species and justifies the development of a specific setup for its capture and immobilization. In this study, we report for the first time the capture and immobilization of gaseous RuO4 within a porous metal-organic framework (UiO-66-NH2). We used specific installation for the production of gaseous RuO4 as well as for the quantification of this gas trapped within the filtering medium. We proved that UiO-66-NH2 has remarkable affinity for RuO4 capture, as this MOF exhibited the worldwide highest RuO4 decontamination factor (DF of 5745), hundreds of times higher than the DF values of sorbents daily used by the nuclear industry (zeolites or activated charcoal). The efficiency of UiO-66-NH2 can be explained by its pore diameters well adapted to the capture and immobilization of RuO4 as well as its conversion into stable RuO2 within the pores. This conversion corresponds to the reactivity of RuO4 with the MOF organic sub-network, leading to the oxidation of terephthalate ligands. As proved by powder X-ray diffraction and NMR techniques, these modifications did not decompose the MOF structure.
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