Electron energy-loss spectroscopy of anomalous plutonium behavior in nuclear waste materials.

Plutonium-enriched layer has been observed in corroded spent uranium oxide fuel (CSNF). These Pu-enriched regions were examined with analytical transmission electron microscopy combined with electron energy-loss spectroscopy (EELS). The enriched region also contained U, Am, Ru, Zr, but only minor enrichment of rare earth elements. The Pu, possibly as Pu(V) according to EELS measurements, was dispersed within re-precipitated uranium oxide (identified as U3O8) nano-crystals between U(VI) secondary phases and the CSNF surface. The U, Pu, and Am enrichment was observed in the corrosion products with tests on different nuclear fuels. This may have implications for the long-term behavior of CSNF under storage in a geologic waste repository. Furthermore, there may be an increased potential for the generation of Pu-bearing colloids from this type of weathered CSNF.

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