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<p>Raman, FTIR, and diffuse reflectance spectroscopy were used to study the auto-radiolytic degradation of <sup>240</sup>Pu and <sup>242</sup>Pu oxalates. The significant differences in the lifetimes of <sup>240</sup>Pu and <sup>242</sup>Pu enabled the differentiation between environmental and radiolytic mechanisms. <sup>240</sup>Pu oxalates were observed to decompose to PuOCO<sub>3</sub> at intermediate times (~ 20&#xa0;weeks) followed by partial conversion to PuO<sub>2</sub> at times greater than one year. Atmospheric oxidation was shown to be the primary decomposition mechanism for <sup>242</sup>Pu(IV) oxalate, and the alpha radiolysis of aquo and oxalate ligands serves as a secondary decomposition mechanism. This study offers a fresh perspective on radiolytic aging, which is crucial for long-term storage applications.</p>

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Radiolytic degradation of 240Plutonium and 242Plutonium oxalates

  • 期刊论文

  • 发表日期：

    2025年12月1日

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  • Jason R. Darvin,
  • Weslee A. Kersey,
  • Eliel Villa-Aleman,
  • Don D. Dick,
  • Thomas C. Shehee,
  • Bryan J. Foley,
  • Austin L. Dorris,
  • Kyle C. Hartig

摘要

Raman, FTIR, and diffuse reflectance spectroscopy were used to study the auto-radiolytic degradation of 240Pu and 242Pu oxalates. The significant differences in the lifetimes of 240Pu and 242Pu enabled the differentiation between environmental and radiolytic mechanisms. 240Pu oxalates were observed to decompose to PuOCO3 at intermediate times (~ 20 weeks) followed by partial conversion to PuO2 at times greater than one year. Atmospheric oxidation was shown to be the primary decomposition mechanism for 242Pu(IV) oxalate, and the alpha radiolysis of aquo and oxalate ligands serves as a secondary decomposition mechanism. This study offers a fresh perspective on radiolytic aging, which is crucial for long-term storage applications.