U-Pu Mixed Oxide Particle Analysis by NAUTILUS and Implications for Next-Generation Verification Challenges.

Precise and accurate measurement of U and Pu isotopes from micrometer-sized particles represents new verification challenges for the International Atomic Energy Agency. The U and Pu isotopes and U-Pu elemental ratio provide valuable information about the intended use, the production process, and the purification process of Pu and mixed oxide (MOX) fuels. We demonstrate the ability to directly measure U and Pu isotopes from MOX fuel particles using the U.S. Naval Research Laboratory's Naval Ultra-Trace Isotope Laboratory's Universal Spectrometer (NAUTILUS). Reactor-grade MOX reference materials with well-characterized U and Pu isotopic composition (e.g., UKMOX10 and UKMOX100) were prepared using standard sample preparation methods for large geometry-secondary ion mass spectrometry (LG-SIMS). The results show that the NAUTILUS can discriminate the 238U1H+ signal from 239Pu+, enabling the accurate measurement of the 240Pu/239Pu ratio for MOX particles within 2σ of the certificate value for U-Pu ratios from 3:1 to 300:1. The accuracy of previously reported LG-SIMS measurements was limited to U-Pu ratios <15:1. Using the NAUTILUS, the 234U/238U, 235U/238U, 236U/238U, 240Pu/239Pu, and 242Pu/239Pu ratios for UKMOX10 and UKMOX100 can all be measured accurately within 2σ of the reference values, directly, without correction. The application of the NAUTILUS to the accurate and precise determination of the elemental and isotopic composition of MOX particles in environmental samples may unravel some emerging verification challenges in international safeguards.