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Fluorite-derived high-entropy ceramic waste form for immobilizing multi-nuclides with multi-valence: a case study of Nb5+ as charge compensator.

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Title: Fluorite-derived high-entropy ceramic waste form for immobilizing multi-nuclides with multi-valence: a case study of Nb5+ as charge compensator.
Authors: Ji, Xiuhua1,2,3 (AUTHOR), Wang, Lielin1,2 (AUTHOR) wanglielin@swust.edu.cn, Ji, Shiyin1,2 (AUTHOR) jishy@swust.edu.cn, Zhang, Sinian3 (AUTHOR), Fang, Shuohai3 (AUTHOR), Xu, Jiaqi3 (AUTHOR), Shih, Kaimin4 (AUTHOR), Liao, Changzhong1,3 (AUTHOR) liaocz29@connect.hku.hk
Source: Ceramics International. May2026:Part A, Vol. 52 Issue 11, p15399-15407. 9p.
Subjects: Pyrochlore, Radioactive waste sites, Ceramics, Radioisotopes, Oxide ceramics
Abstract: Given its significant radiological hazards to public safety, high-level radioactive waste (HLW) must be immobilized into stable waste forms for long-term geological disposal. High-entropy ceramics have garnered significant research interest for their unique ability to simultaneously immobilize multiple radionuclides. In this work, aiming to immobilize multivalent actinides (simulated by REEs) using Nb as charge compensator, a series of novel high-entropy zirconolite samples were successfully synthesized via high temperature solid-state reaction. The compositions were designed as CaZr 1-5x REE 5x Ti 2-5x Nb 5x O 7 (REE = Nd, Sm, Gd, Ho, Yb; x = 0.02, 0.05, 0.10, 0.15, 0.20) and CaZr 1-6x Ce x REE 5x Ti 2-5x Nb 5x O 7 (REE = Nd, Sm, Gd, Ho, Yb; x = 0.02, 0.04, 0.08, 0.10, 0.15). The powder XRD, back-scattered SEM and Raman characterization results revealed a phase evolution following the zirconolite-2M→zirconolite-4M→pyrochlore pathway in those two-type compositions. For CaZr 1-5x REE 5x Ti 2-5x Nb 5x O 7 type high-entropy ceramics, a small amount of perovskite was observed alongside zirconolite. A single-phase pyrochlore structure was obtained at x ≥ 0.10. For compositions with CaZr 1-6x Ce x REE 5x Ti 2-5x Nb 5x O 7 , trace perovskite phase was detected throughout the solid-solution range, which may be attributed to the fluctuations of Ce oxidation state. Interestingly, the Raman spectra displayed signification difference in difference excitation wavelength. The reasons should be attributed to the resonant enhancement or suppression of specific modes due to elemental doping and the contribution from background fluorescence. This study revealed that the structural adaptability of fluorite-derived high-entropy ceramics makes them well-suited for the immobilization of high-level waste, particularly for actinides. [ABSTRACT FROM AUTHOR]
Copyright of Ceramics International is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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DbLabel: Engineering Source
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  Data: Fluorite-derived high-entropy ceramic waste form for immobilizing multi-nuclides with multi-valence: a case study of Nb5+ as charge compensator.
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  Data: <searchLink fieldCode="JN" term="%22Ceramics+International%22">Ceramics International</searchLink>. May2026:Part A, Vol. 52 Issue 11, p15399-15407. 9p.
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  Data: <searchLink fieldCode="DE" term="%22Pyrochlore%22">Pyrochlore</searchLink><br /><searchLink fieldCode="DE" term="%22Radioactive+waste+sites%22">Radioactive waste sites</searchLink><br /><searchLink fieldCode="DE" term="%22Ceramics%22">Ceramics</searchLink><br /><searchLink fieldCode="DE" term="%22Radioisotopes%22">Radioisotopes</searchLink><br /><searchLink fieldCode="DE" term="%22Oxide+ceramics%22">Oxide ceramics</searchLink>
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  Label: Abstract
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  Data: Given its significant radiological hazards to public safety, high-level radioactive waste (HLW) must be immobilized into stable waste forms for long-term geological disposal. High-entropy ceramics have garnered significant research interest for their unique ability to simultaneously immobilize multiple radionuclides. In this work, aiming to immobilize multivalent actinides (simulated by REEs) using Nb as charge compensator, a series of novel high-entropy zirconolite samples were successfully synthesized via high temperature solid-state reaction. The compositions were designed as CaZr 1-5x REE 5x Ti 2-5x Nb 5x O 7 (REE = Nd, Sm, Gd, Ho, Yb; x = 0.02, 0.05, 0.10, 0.15, 0.20) and CaZr 1-6x Ce x REE 5x Ti 2-5x Nb 5x O 7 (REE = Nd, Sm, Gd, Ho, Yb; x = 0.02, 0.04, 0.08, 0.10, 0.15). The powder XRD, back-scattered SEM and Raman characterization results revealed a phase evolution following the zirconolite-2M→zirconolite-4M→pyrochlore pathway in those two-type compositions. For CaZr 1-5x REE 5x Ti 2-5x Nb 5x O 7 type high-entropy ceramics, a small amount of perovskite was observed alongside zirconolite. A single-phase pyrochlore structure was obtained at x ≥ 0.10. For compositions with CaZr 1-6x Ce x REE 5x Ti 2-5x Nb 5x O 7 , trace perovskite phase was detected throughout the solid-solution range, which may be attributed to the fluctuations of Ce oxidation state. Interestingly, the Raman spectra displayed signification difference in difference excitation wavelength. The reasons should be attributed to the resonant enhancement or suppression of specific modes due to elemental doping and the contribution from background fluorescence. This study revealed that the structural adaptability of fluorite-derived high-entropy ceramics makes them well-suited for the immobilization of high-level waste, particularly for actinides. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
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  Data: <i>Copyright of Ceramics International is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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RecordInfo BibRecord:
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      – Type: doi
        Value: 10.1016/j.ceramint.2026.02.145
    Languages:
      – Code: eng
        Text: English
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        PageCount: 9
        StartPage: 15399
    Subjects:
      – SubjectFull: Pyrochlore
        Type: general
      – SubjectFull: Radioactive waste sites
        Type: general
      – SubjectFull: Ceramics
        Type: general
      – SubjectFull: Radioisotopes
        Type: general
      – SubjectFull: Oxide ceramics
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      – TitleFull: Fluorite-derived high-entropy ceramic waste form for immobilizing multi-nuclides with multi-valence: a case study of Nb5+ as charge compensator.
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              M: 05
              Text: May2026:Part A
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