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<p>Actinide and lanthanide binary nitrides (<i>An</i>N, <i>Ln</i>N), are isostructural cubic compounds relevant to next-generation nuclear fuels which require detailed understanding regarding their oxidative degradation for safe disposal, yet a systematic comparative description remains. Herein, the room- and high-temperature oxidation behaviour of U<sup>3+</sup>N and <i>Ln</i><sup><i>3+</i></sup>N (<i>Ln</i> = Pr, Nd, Gd, Tb, Dy, Ho, Tm and Lu) compounds is examined via a combination of X-ray diffraction, electron microscopy, thermogravimetric, and X-ray absorption spectroscopy analysis. At room temperature, UN was found to undergo an oxygen mediated oxidising mechanism, which contrasted chemically and microstructurally to the <i>Ln</i>N’s<sub>,</sub> which followed a consistent hydrolysis mechanism. At high temperature, more congruent behaviour is determined with direct occurrence of oxide products, where the onset temperature of oxidation was found to correlate with the ionic radii of examined <i>Ln</i>/U cations. The results provide insight into the behaviour of these compounds in UN-based spent fuel, particularly phase separation variability and incongruent behaviour during inadvertent oxidation.</p>

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The ambient- and high-temperature oxidation behaviour of U3+N and Ln3+N compounds relevant to spent nuclear fuel

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月16日

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  • Pascal Uhlemann,
  • Emily M. Reynolds,
  • Martina Klinkenberg,
  • Damien Prieur,
  • Christian Schreinemachers,
  • Philip Kegler,
  • Celina Erven,
  • Sven M. Schenk,
  • Joerg Göttlicher,
  • Ralph Steininger,
  • Mary Blankenship,
  • Lothar Weinhardt,
  • Nina Huittinen,
  • Peter Höhn,
  • Tonya Vitova,
  • Giuseppe Modolo,
  • Gabriel L. Murphy

摘要

Actinide and lanthanide binary nitrides (AnN, LnN), are isostructural cubic compounds relevant to next-generation nuclear fuels which require detailed understanding regarding their oxidative degradation for safe disposal, yet a systematic comparative description remains. Herein, the room- and high-temperature oxidation behaviour of U3+N and Ln3+N (Ln = Pr, Nd, Gd, Tb, Dy, Ho, Tm and Lu) compounds is examined via a combination of X-ray diffraction, electron microscopy, thermogravimetric, and X-ray absorption spectroscopy analysis. At room temperature, UN was found to undergo an oxygen mediated oxidising mechanism, which contrasted chemically and microstructurally to the LnN’s, which followed a consistent hydrolysis mechanism. At high temperature, more congruent behaviour is determined with direct occurrence of oxide products, where the onset temperature of oxidation was found to correlate with the ionic radii of examined Ln/U cations. The results provide insight into the behaviour of these compounds in UN-based spent fuel, particularly phase separation variability and incongruent behaviour during inadvertent oxidation.