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Peer-reviewedCC BYInorganic chemistry

Post-Mortem Characterization of Cerium Speciation in Molten Calcium Chloride.

  1. 1Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, California94550, United States.
  2. 2Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico87545, United States.

Abstract

Advancing radiochemistry and nuclear materials science requires understanding actinide interactions with molten salts, which are used in next-generation nuclear reactors and for processing of actinides to recover useful fissile material. Understanding chemical interactions of actinides with molten salts has been limited by challenges in developing spectroscopic and X-ray techniques that are compatible with the high temperatures necessary to study molten salts. In this work, interactions of CeO2 (serving as a nonradioactive surrogate for uranium and plutonium) with CaCl2 are characterized following heating. Scanning electron microscopy indicates CeO2 morphological changes from small (<1 μm) particles to 3-5 μm sheets. Powder X-ray diffraction and infrared and Raman spectroscopies show the formation of CeOCl at higher (850-1050 °C) temperatures. In the absence of a chemical reducing agent, it was found that a high-temperature, low-oxygen environment is the key to the formation of oxychloride and that oxychloride formation is inhibited by annealing the CeO2 starting material. Lastly, thermal analysis revealed lowering of the melting point of CaCl2 after heating with CeO2. In all, this work identifies applicable spectroscopic techniques to target studies of heavy elements in molten salt environments and highlights the relationship between chemical speciation and melting behavior, a key thermophysical property.

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BibTeX
@article{kelly2026postmortem,
  title = {{Post-Mortem Characterization of Cerium Speciation in Molten Calcium Chloride.}},
  author = {Sheridon N Kelly and Alfred Amon and Maryline G Ferrier and Karla A Erickson and L Eddy Banks and Marisa J Monreal and Bradley C Childs},
  journal = {Inorganic chemistry},
  year = {2026},
  month = sep,
  doi = {10.1021/acs.inorgchem.6c02415},
  url = {https://europepmc.org/article/MED/42916193},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Post-Mortem Characterization of Cerium Speciation in Molten Calcium Chloride.
AU  - Sheridon N Kelly
AU  - Alfred Amon
AU  - Maryline G Ferrier
AU  - Karla A Erickson
AU  - L Eddy Banks
AU  - Marisa J Monreal
AU  - Bradley C Childs
PY  - 2026
DA  - 2026/09/01
JO  - Inorganic chemistry
DO  - 10.1021/acs.inorgchem.6c02415
UR  - https://europepmc.org/article/MED/42916193
AB  - Advancing radiochemistry and nuclear materials science requires understanding actinide interactions with molten salts, which are used in next-generation nuclear reactors and for processing of actinides to recover useful fissile material. Understanding chemical interactions of actinides with molten salts has been limited by challenges in developing spectroscopic and X-ray techniques that are compatible with the high temperatures necessary to study molten salts. In this work, interactions of CeO2 (serving as a nonradioactive surrogate for uranium and plutonium) with CaCl2 are characterized following heating. Scanning electron microscopy indicates CeO2 morphological changes from small (<1 μm) particles to 3-5 μm sheets. Powder X-ray diffraction and infrared and Raman spectroscopies show the formation of CeOCl at higher (850-1050 °C) temperatures. In the absence of a chemical reducing agent, it was found that a high-temperature, low-oxygen environment is the key to the formation of oxychloride and that oxychloride formation is inhibited by annealing the CeO2 starting material. Lastly, thermal analysis revealed lowering of the melting point of CaCl2 after heating with CeO2. In all, this work identifies applicable spectroscopic techniques to target studies of heavy elements in molten salt environments and highlights the relationship between chemical speciation and melting behavior, a key thermophysical property.
SN  - 0020-1669
SN  - 1520-510X
ER  -