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<p>Monoclinic zirconia (<i>m-</i>ZrO<sub>2</sub>) forms on the internal surface of nuclear fuel Zircaloy cladding, acting as a critical barrier against radionuclide release at the fuel-cladding interface. However, the incorporation of minor actinide elements like americium in <i>m-</i>ZrO₂ and resultant structural chemistry remains poorly understood. Using a combination of diffraction and high-resolution X-ray spectroscopic techniques, we have examined <i>m-</i>ZrO<sub>2</sub> with 5 mol% Am doping. We show Am enters <i>m-</i>ZrO<sub>2</sub> tetravalently, where its solubility is approximately 1.0 mol%, <i>m</i>-(Am<sup>4+</sup><sub>0.011(7)</sub>Zr<sup>4+</sup><sub>0.989(7)</sub>)O<sub>2</sub>, attributed to the large Am<sup>4+</sup> cation, where excess Am, that is predominantly trivalent, adopts a C-type (Am<sup>4+/3+</sup><sub>1-x</sub>Zr<sup>4+</sup><sub>x</sub>)<sub>2</sub>O<sub>3+x</sub> phase in space group <i>Ia</i>-3. The known reversible high temperature phase transformation of <i>m-</i>ZrO<sub>2</sub> to tetragonal is further shown to be reduced from 1150 <sup>o</sup>C to 1050 <sup>o</sup>C via Am<sup>4+</sup> incorporation. The investigation provides critical insight into the chemical reactivity and speciation of minor actinide elements with nuclear fuel cladding related <i>m-</i>ZrO₂.</p><p></p>

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Structural and chemical insights on the incorporation of americium into zircaloy-derived monoclinic zirconia

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月26日

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  • Gabriel L. Murphy,
  • Sara Gilson,
  • Karin Popa,
  • Damien Prieur,
  • Sven M. Schenk,
  • Sorin-Octavian Valu,
  • Harry Ramanantoanina,
  • Tim Prüßmann,
  • Tonya Vitova,
  • Kathy Dardenne,
  • Jörg Rothe,
  • Jean-Yves Colle,
  • Olaf Walter,
  • Nina Huittinen

摘要

Monoclinic zirconia (m-ZrO2) forms on the internal surface of nuclear fuel Zircaloy cladding, acting as a critical barrier against radionuclide release at the fuel-cladding interface. However, the incorporation of minor actinide elements like americium in m-ZrO₂ and resultant structural chemistry remains poorly understood. Using a combination of diffraction and high-resolution X-ray spectroscopic techniques, we have examined m-ZrO2 with 5 mol% Am doping. We show Am enters m-ZrO2 tetravalently, where its solubility is approximately 1.0 mol%, m-(Am4+0.011(7)Zr4+0.989(7))O2, attributed to the large Am4+ cation, where excess Am, that is predominantly trivalent, adopts a C-type (Am4+/3+1-xZr4+x)2O3+x phase in space group Ia-3. The known reversible high temperature phase transformation of m-ZrO2 to tetragonal is further shown to be reduced from 1150 oC to 1050 oC via Am4+ incorporation. The investigation provides critical insight into the chemical reactivity and speciation of minor actinide elements with nuclear fuel cladding related m-ZrO₂.