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Related Experiment Videos

Oxidation of plutonium dioxide.

Pavel A Korzhavyi1, Levente Vitos, David A Andersson

  • 1Applied Materials Physics, Department of Materials Science and Engineering, Royal Institute of Technology (KTH), SE-100 44 Stockholm, Sweden. pavel@met.kth.se

Nature Materials
|March 23, 2004
PubMed
Summary

Plutonium dioxide unexpectedly reacts with water to form higher oxides. Theoretical analysis reveals these reactions require energy but can occur via radiolysis products like hydrogen peroxide.

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Area of Science:

  • Nuclear chemistry
  • Actinide element physics and chemistry

Background:

  • Plutonium dioxide (PuO2) was considered the highest stable oxide of plutonium.
  • Recent experiments show PuO2 reacts with water to form higher oxides (up to PuO2.27).

Purpose of the Study:

  • To theoretically analyze the unexpected formation of higher plutonium oxides.
  • To understand the thermodynamic feasibility of PuO2 oxidation by water and oxygen.

Main Methods:

  • Density functional theory (DFT) calculations for total energies.
  • Integration of DFT results with established thermodynamic data.

Main Results:

  • Reactions of PuO2 with O2 or H2O to form PuO(2+delta) are endothermic, requiring energy input.
  • Higher plutonium oxides (PuO2+delta) can form as intermediate products through reactions with water radiolysis products, such as hydrogen peroxide (H2O2).

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Conclusions:

  • The formation of higher plutonium oxides is thermodynamically challenging under direct reaction with O2 or H2O.
  • Radiolysis products of water provide a viable pathway for the formation of higher plutonium oxides, explaining experimental observations.