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Article Abstract
The separation of radionuclide americium (Am) is a crucial challenge in the reprocessing of spent nuclear fuel, due to the complex speciation. Selective coordination of hexavalent americium [Am (VI)] with covalent organic frameworks (COFs) has emerged as a promising strategy to address this issue. In this work, we employed first-principles simulations combined with density functional theory (DFT) to investigate the adsorption stability of COF (PyN-DAB) for the linear americyl ion AmO22+. Our results demonstrate that COFs can effectively and stably coordinate with Am (VI), highlighting their potential for Am separation. Furthermore, we explored the high-oxidation-state model of AmO22+ complexes with the PyN-DAB ligand to elucidate the underlying microscopic interaction mechanisms between AmO22+ and the PyN-DAB monomer. Comprehensive analyses revealed a strong attraction between the PyN-DAB and AmO22+, which is attributed to the synergistic effects of electrostatic interactions, orbital interactions, and π-electron-rich aromatic rings within the PyN-DAB framework. These findings not only provide fundamental insights into the Am separation process but also offer a novel perspective on the potential applications of COFs in the efficient extraction of actinides. Thus, this study contributes to the ongoing efforts to develop advanced materials for nuclear fuel reprocessing and waste management.
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Theoretical investigation into the interaction mechanism of hexavalent americium with covalent organic framework (PyN-DAB).
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State Key Laboratory of Quantum Optics Technologies and Devices, School of Physics and Electronics Engineering, Institute of Laser Spectroscopy, Shanxi University, Taiyuan 030006, China.
The separation of radionuclide americium (Am) is a crucial challenge in the reprocessing of spent nuclear fuel, due to the complex speciation. Selective coordination of hexavalent americium [Am (VI)] with covalent organic frameworks (COFs) has emerged as a promising strategy to address this issue. In this work, we employed first-principles simulations combined with density functional theory (DFT) to investigate the adsorption stability of COF (PyN-DAB) for the linear americyl ion AmO22+.
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State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou, China.
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Nuclear Engineering and Science Center, Texas A&M University, College Station, TX 77843, USA.
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July 2019
Department of Chemistry and Biochemistry , California State University Long Beach, 1250 Bellflower Boulevard , Long Beach California 90840-9507 , United States.
The recent development of facile methods to oxidize trivalent americium to its higher valence states holds promise for the discovery of new chemistries and critical insight into the behavior of the 5f electrons. However, progress in understanding high-valent americium chemistry has been hampered by americium's inherent ionizing radiation field and its concomitant effects on americium redox chemistry. Any attempt to understand high-valent americium reduction and/or disproportionation must account for the effects of these radiolytic processes.
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