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Yanmei He. Portrait.

Yanmei He

Postdoctoral fellow

Yanmei He. Portrait.

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

Author

  • Yibo Wang
  • Kun Yang
  • Feida Chen
  • Xianlin Qu
  • Yanmei He
  • Daniu Han
  • Xiaobin Tang

Summary, in English

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.

Department/s

  • LU Profile Area: Light and Materials
  • LTH Profile Area: Nanoscience and Semiconductor Technology
  • Chemical Physics
  • NanoLund: Centre for Nanoscience

Publishing year

2025-02-24

Language

English

Pages

3178-3187

Publication/Series

Inorganic Chemistry

Volume

64

Issue

7

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Inorganic Chemistry

Status

Published

ISBN/ISSN/Other

  • ISSN: 0020-1669