Abstract
Isotope ratio analysis of nuclear materials in individual particles is of great importance for nuclear safeguards. Although secondary ion mass spectrometry (SIMS) and thermal ionization mass spectrometry (TIMS) are utilized for the analysis of individual uranium particles, few studies were conducted for the analysis of individual uranium-plutonium mixed oxide particles. In this study, we applied SIMS and inductively coupled plasma mass spectrometry (ICP-MS) to the isotope ratio analysis of individual U-Pu mixed oxide particles. In the analysis of individual U-Pu particles prepared from mixed solution of uranium and plutonium standard reference materials, accurate 235 U/ 238 U, 240 Pu/ 239 Pu and 242 Pu/ 239 Pu isotope ratios were obtained with both methods. However, accurate analysis of 241 Pu/ 239 Pu isotope ratio was impossible, due to the interference of the 241 Am peak to the 241 Pu peak. In addition, it was indicated that the interference of the 238 UH peak to the 239 Pu peak has a possibility to prevent accurate analysis of plutonium isotope ratios. These problems would be avoided by a combination of ICP-MS and chemical separation of uranium, plutonium and americium in individual U-Pu particles.
Highlights
Mass spectrometry has a crucial role in nuclear safeguards
We developed a technique by a combination of particle manipulation under scanning electron microscope (SEM) and isotope ratio analysis with secondary ion mass spectrometry (SIMS).[5]
In a previous study,[14] we developed an experimental technique for individual plutonium particles, which included particle manipulation, dissolution and chemical separation of plutonium and americium for subsequent isotope ratio analysis with inductively coupled plasma mass spectrometry (ICP-MS)
Summary
Isotope ratio analysis of individual uranium particles in environmental samples taken at nuclear facilities is performed to verify the absence of undeclared nuclear activities related to uranium enrichment and production of nuclear weapons.[1,2] For this purpose, two kinds of analytical techniques are mainly used, i.e., secondary ion mass spectrometry (SIMS) and thermal ionization mass spectrometry (TIMS) combined with a fission track method.[3,4,5,6,7,8,9,10,11,12] The SIMS allows us to analyze samples and rapidly. In order to overcome this problem, a large geometry SIMS instrument with high mass resolution was used to separate peaks of uranium ions and molecular ions.[7] As the result, accurate isotope ratio results were acquired in the analysis of swipe samples taken at nuclear facilities by using the instrument. The particle manipulation allowed us to transfer only uranium particles for subsequent
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