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Structural Stability and Photoluminescence Property of Cs2UCl6 Single Crystal Derived from Spent Nuclear Fuel

Wang, Yibo LU ; Yang, Kun ; Chen, Feida ; Qu, Xianlin ; He, Yanmei LU ; Han, Daniu and Tang, Xiaobin (2025) In Inorganic Chemistry 64(7). p.3178-3187
Abstract

The recycling and reuse of trace uranium from spent nuclear fuel is of great significance for the safety management of the nuclear fuel cycle. However, stabilization of low-valent uranium has always been a challenge due to the ultraoxidizable nature of uranium ions, which remains relatively uncharted territory in spent fuel treatment. In the current study, U4+ was immobilized in Cs2UCl6 single crystal with a perovskite structure from uranyl under a strong acidic environment. A comprehensive and detailed understanding of Cs2UCl6 at the atomic scale has been achieved by combining density functional theory (DFT) with high-resolution integrated differential phase contrast scanning... (More)

The recycling and reuse of trace uranium from spent nuclear fuel is of great significance for the safety management of the nuclear fuel cycle. However, stabilization of low-valent uranium has always been a challenge due to the ultraoxidizable nature of uranium ions, which remains relatively uncharted territory in spent fuel treatment. In the current study, U4+ was immobilized in Cs2UCl6 single crystal with a perovskite structure from uranyl under a strong acidic environment. A comprehensive and detailed understanding of Cs2UCl6 at the atomic scale has been achieved by combining density functional theory (DFT) with high-resolution integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM) imaging, which was captured by utilizing Cs-corrected TEM for the first time. Furthermore, the results obtained from X-ray excitation and the photoexcitation effects produced by PL at 280, 330, and 360 nm provide compelling evidence for the ability of U4+ to form excitable bands around the Fermi level. The as-synthesized Cs2UCl6 demonstrates excellent thermal stability above 275 °C, as evidenced by in situ Raman spectroscopy and thermogravimetric analysis, while a degradation pathway initiated by CsCl upon exposure to water vapor was revealed by synchrotron X-ray diffraction. Thermal and chemical stability can be further elevated by consolidating it into a metal−organic framework (MOF) via hot pressing. The current study provides a promising strategy to reuse and functionalize the spent nuclear fuel.

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author
; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Inorganic Chemistry
volume
64
issue
7
pages
10 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85218604285
  • pmid:39935380
ISSN
0020-1669
DOI
10.1021/acs.inorgchem.4c04076
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2025 American Chemical Society.
id
7aa4deef-c370-4101-beb3-4f6192424d71
date added to LUP
2025-06-20 10:35:18
date last changed
2025-07-18 13:47:55
@article{7aa4deef-c370-4101-beb3-4f6192424d71,
  abstract     = {{<p>The recycling and reuse of trace uranium from spent nuclear fuel is of great significance for the safety management of the nuclear fuel cycle. However, stabilization of low-valent uranium has always been a challenge due to the ultraoxidizable nature of uranium ions, which remains relatively uncharted territory in spent fuel treatment. In the current study, U<sup>4+</sup> was immobilized in Cs<sub>2</sub>UCl<sub>6</sub> single crystal with a perovskite structure from uranyl under a strong acidic environment. A comprehensive and detailed understanding of Cs<sub>2</sub>UCl<sub>6</sub> at the atomic scale has been achieved by combining density functional theory (DFT) with high-resolution integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM) imaging, which was captured by utilizing Cs-corrected TEM for the first time. Furthermore, the results obtained from X-ray excitation and the photoexcitation effects produced by PL at 280, 330, and 360 nm provide compelling evidence for the ability of U<sup>4+</sup> to form excitable bands around the Fermi level. The as-synthesized Cs<sub>2</sub>UCl<sub>6</sub> demonstrates excellent thermal stability above 275 °C, as evidenced by in situ Raman spectroscopy and thermogravimetric analysis, while a degradation pathway initiated by CsCl upon exposure to water vapor was revealed by synchrotron X-ray diffraction. Thermal and chemical stability can be further elevated by consolidating it into a metal−organic framework (MOF) via hot pressing. The current study provides a promising strategy to reuse and functionalize the spent nuclear fuel.</p>}},
  author       = {{Wang, Yibo and Yang, Kun and Chen, Feida and Qu, Xianlin and He, Yanmei and Han, Daniu and Tang, Xiaobin}},
  issn         = {{0020-1669}},
  language     = {{eng}},
  month        = {{02}},
  number       = {{7}},
  pages        = {{3178--3187}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Inorganic Chemistry}},
  title        = {{Structural Stability and Photoluminescence Property of Cs<sub>2</sub>UCl<sub>6</sub> Single Crystal Derived from Spent Nuclear Fuel}},
  url          = {{http://dx.doi.org/10.1021/acs.inorgchem.4c04076}},
  doi          = {{10.1021/acs.inorgchem.4c04076}},
  volume       = {{64}},
  year         = {{2025}},
}