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High-entropy ceramic strategy for immobilizing multi-radionuclides in zirconolite structure.

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Title: High-entropy ceramic strategy for immobilizing multi-radionuclides in zirconolite structure.
Authors: Wang, Keshen1 (AUTHOR), Fang, Shuohai1 (AUTHOR), Luo, Hui1 (AUTHOR), Yu, Lu1 (AUTHOR), Li, Dongmei1 (AUTHOR), Wu, Jiani1 (AUTHOR), Yin, Xiangbiao1,2 (AUTHOR) yinxb@usc.edu.cn, Yang, Wenchao1 (AUTHOR), Ma, Shengshou3 (AUTHOR), Shih, Kaimin3 (AUTHOR), Liao, Changzhong1,3 (AUTHOR) liaocz29@connect.hku.hk
Source: Ceramics International. May2026:Part B, Vol. 52 Issue 12, p20417-20425. 9p.
Subjects: Radioactive waste disposal, Oxide ceramics, Zirconium, Phase equilibrium, X-ray diffraction, Radioactive waste sites, Doping agents (Chemistry), Radioisotopes
Abstract: Effective high-level radioactive waste (HLW) immobilization is crucial for advancing nuclear energy. Zirconolite ceramics are a key material, known for their stability and durability. This study explores the potential of high-entropy zirconolite ceramics for disposing of multi-radionuclide high-level radioactive waste. A series of Ca 1-5x REE 5x ZrTi 2-5x Al 5x O 7 (REE-Al), Ca 1-5x REE 5x ZrTi 2-5x Fe 5x O 7 (REE-Fe) and Ca 1-5x REE 5x ZrTi 2-5x Al 2.5x Fe 2.5x O 7 (REE-Fe-Al) (REE = Nd, Sm, Gd, Ho, Yb; x = 0.05-0.20) were synthesized and characterized using XRD, SEM, XPS, and XAS techniques. Results show that zirconolite-2M remains the dominant phase up to x = 0.15. At higher doping levels (x ≥ 0.18), secondary phases such as cubic zirconia, baddeleyite in the REE-Al samples. In REE-Fe and REE-Al-Fe samples, both zirconolite-2M and zirconolite-3O can form, with a phase transformation from 2M to 3O occurring at x ≥ 0.18. XPS results confirm that the chemical states of all elements remain stable after high-temperature sintering. XANES analysis indicates that Al3+ ions substitute both Ti sites within the TiO 5 and TiO 6 coordination environments, with a preference for occupying the TiO 5 sites. EXAFS analysis indicates that while Zr substitution for Ca is minimal at low dopant levels, a substantial amount of Zr starts occupying Ca sites as doping concentration increases. This work demonstrates that high-entropy strategies dramatically enhance the compositional flexibility of zirconolite, enabling simultaneous incorporation of diverse charge-compensating dopants while maintaining structural and phase stability. [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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  Label: Title
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  Data: High-entropy ceramic strategy for immobilizing multi-radionuclides in zirconolite structure.
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  Data: <searchLink fieldCode="AR" term="%22Wang%2C+Keshen%22">Wang, Keshen</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Fang%2C+Shuohai%22">Fang, Shuohai</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Luo%2C+Hui%22">Luo, Hui</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Yu%2C+Lu%22">Yu, Lu</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Li%2C+Dongmei%22">Li, Dongmei</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Wu%2C+Jiani%22">Wu, Jiani</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Yin%2C+Xiangbiao%22">Yin, Xiangbiao</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<i> yinxb@usc.edu.cn</i><br /><searchLink fieldCode="AR" term="%22Yang%2C+Wenchao%22">Yang, Wenchao</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Ma%2C+Shengshou%22">Ma, Shengshou</searchLink><relatesTo>3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Shih%2C+Kaimin%22">Shih, Kaimin</searchLink><relatesTo>3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Liao%2C+Changzhong%22">Liao, Changzhong</searchLink><relatesTo>1,3</relatesTo> (AUTHOR)<i> liaocz29@connect.hku.hk</i>
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  Data: <searchLink fieldCode="JN" term="%22Ceramics+International%22">Ceramics International</searchLink>. May2026:Part B, Vol. 52 Issue 12, p20417-20425. 9p.
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  Data: <searchLink fieldCode="DE" term="%22Radioactive+waste+disposal%22">Radioactive waste disposal</searchLink><br /><searchLink fieldCode="DE" term="%22Oxide+ceramics%22">Oxide ceramics</searchLink><br /><searchLink fieldCode="DE" term="%22Zirconium%22">Zirconium</searchLink><br /><searchLink fieldCode="DE" term="%22Phase+equilibrium%22">Phase equilibrium</searchLink><br /><searchLink fieldCode="DE" term="%22X-ray+diffraction%22">X-ray diffraction</searchLink><br /><searchLink fieldCode="DE" term="%22Radioactive+waste+sites%22">Radioactive waste sites</searchLink><br /><searchLink fieldCode="DE" term="%22Doping+agents+%28Chemistry%29%22">Doping agents (Chemistry)</searchLink><br /><searchLink fieldCode="DE" term="%22Radioisotopes%22">Radioisotopes</searchLink>
– Name: Abstract
  Label: Abstract
  Group: Ab
  Data: Effective high-level radioactive waste (HLW) immobilization is crucial for advancing nuclear energy. Zirconolite ceramics are a key material, known for their stability and durability. This study explores the potential of high-entropy zirconolite ceramics for disposing of multi-radionuclide high-level radioactive waste. A series of Ca 1-5x REE 5x ZrTi 2-5x Al 5x O 7 (REE-Al), Ca 1-5x REE 5x ZrTi 2-5x Fe 5x O 7 (REE-Fe) and Ca 1-5x REE 5x ZrTi 2-5x Al 2.5x Fe 2.5x O 7 (REE-Fe-Al) (REE = Nd, Sm, Gd, Ho, Yb; x = 0.05-0.20) were synthesized and characterized using XRD, SEM, XPS, and XAS techniques. Results show that zirconolite-2M remains the dominant phase up to x = 0.15. At higher doping levels (x ≥ 0.18), secondary phases such as cubic zirconia, baddeleyite in the REE-Al samples. In REE-Fe and REE-Al-Fe samples, both zirconolite-2M and zirconolite-3O can form, with a phase transformation from 2M to 3O occurring at x ≥ 0.18. XPS results confirm that the chemical states of all elements remain stable after high-temperature sintering. XANES analysis indicates that Al3+ ions substitute both Ti sites within the TiO 5 and TiO 6 coordination environments, with a preference for occupying the TiO 5 sites. EXAFS analysis indicates that while Zr substitution for Ca is minimal at low dopant levels, a substantial amount of Zr starts occupying Ca sites as doping concentration increases. This work demonstrates that high-entropy strategies dramatically enhance the compositional flexibility of zirconolite, enabling simultaneous incorporation of diverse charge-compensating dopants while maintaining structural and phase stability. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  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.2026.03.135
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      – Code: eng
        Text: English
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        PageCount: 9
        StartPage: 20417
    Subjects:
      – SubjectFull: Radioactive waste disposal
        Type: general
      – SubjectFull: Oxide ceramics
        Type: general
      – SubjectFull: Zirconium
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      – SubjectFull: Phase equilibrium
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      – SubjectFull: X-ray diffraction
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      – SubjectFull: Radioactive waste sites
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      – SubjectFull: Doping agents (Chemistry)
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      – SubjectFull: Radioisotopes
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      – TitleFull: High-entropy ceramic strategy for immobilizing multi-radionuclides in zirconolite structure.
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              M: 05
              Text: May2026:Part B
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              Y: 2026
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