Simultaneous determination of plutonium and uranium isotope ratios in individual plutonium–uranium mixed particles by thermal ionization mass spectrometry

Lee, Chi-Gyu; Suzuki, D.; Saito‐Kokubu, Yoko; Esaka, Fumitaka; Magara, Masaaki; Kimura, Takaumi

doi:10.1016/j.ijms.2012.02.006

Cited by 25 publications

(19 citation statements)

References 16 publications

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“…Degassing involves resistively heating the filaments under high vacuum for a specified duration of time. Degassing generally is performed to reduce isobaric interferences and background signals that arise from contaminants within the rhenium filaments [30, 31]. Filament contaminants are volatilized during the degassing treatment due to the high temperature and ultralow pressure.…”

Section: Introductionmentioning

confidence: 99%

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Ambient aging of rhenium filaments used in thermal ionization mass spectrometry: Growth of oxo-rhenium crystallites and anti-aging strategies

Mannion

Wellons

Shick

et al. 2017

Heliyon

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Degassing is a common preparation technique for rhenium filaments used for thermal ionization mass spectrometric analysis of actinides, including plutonium. Although optimization studies regarding degassing conditions have been reported, little work has been done to characterize filament aging after degassing. In this study, the effects of filament aging after degassing were explored to determine a “shelf-life” for degassed rhenium filaments, and methods to limit filament aging were investigated. Zone-refined rhenium filaments were degassed by resistance heating under high vacuum before exposure to ambient atmosphere for up to 2 months. After degassing the nucleation and preferential growth of oxo-rhenium crystallites on the surface of polycrystalline rhenium filaments was observed by atomic force microscopy and scanning electron microscopy (SEM). Compositional analysis of the crystallites was conducted using SEM-Raman spectroscopy and SEM energy dispersive X-ray spectroscopy, and grain orientation at the metal surface was investigated by electron back-scatter diffraction mapping. Spectra collected by SEM-Raman suggest crystallites are composed primarily of perrhenic acid. The relative extent of growth and crystallite morphology were found to be grain dependent and affected by the dissolution of carbon into filaments during annealing (often referred to as carbonization or carburization). Crystallites were observed to nucleate in region specific modes and grow over time through transfer of material from the surface. Factors most likely to affect the rates of crystallite growth include rhenium substrate properties such as grain size, orientation, levels of dissolved carbon, and relative abundance of defect sites; as well as environmental factors such as length of exposure to oxygen and relative humidity. Thin (∼180 nm) hydrophobic films of poly(vinylbenzyl chloride) were found to slow the growth of oxo-rhenium crystallites on the filament surfaces and may serve as an alternative carbon source for filament carburization.

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Section: Introductionmentioning

confidence: 99%

“…It has been estimated that filaments reach ∼1500 °C at a current of 3.5 A [32]. In the case of plutonium analyses, it can be expected that filament temperatures reached during degassing are >1500 °C [30, 40, 41]. …”

Section: Introductionmentioning

confidence: 99%

Ambient aging of rhenium filaments used in thermal ionization mass spectrometry: Growth of oxo-rhenium crystallites and anti-aging strategies

Mannion

Wellons

Shick

et al. 2017

Heliyon

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“…In particular, the characterization of individual micron-sized particles in environmental samples taken at nuclear facilities is useful for revealing undeclared nuclear activities. For example, analytical methods to determine plutonium isotope ratios in individual particles have been developed with thermal ionization mass spectrometry (TIMS) and inductively coupled plasma mass spectrometry (ICP-MS) (Esaka et al, 2010;Lee et al, 2012;Miyamoto et al, 2013;Shinonaga et al, 2009;Suzuki et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

“…Therefore, several analytical techniques have been developed to characterize U-Pu mixed samples (Esaka et al, 2011;Lee et al, 2012;Ranebo et al, 2010;Suzuki et al, 2012), which are also important for nuclear safeguards and forensics. In several cases, complex chemical separation processes must be conducted prior to analysis of the uranium and plutonium isotope ratios in U-Pu mixed samples with TIMS and ICP-MS.…”

Section: Introductionmentioning

confidence: 99%

Direct isotope ratio analysis of individual uranium–plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry

Suzuki

Esaka

Miyamoto

et al. 2015

Applied Radiation and Isotopes

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“…7,8,10 Moreover, differences in the evaporation temperatures of the elements allows them to be separated as a function of time. 15 For example, plutonium oxide (PuO 2 ) melts and evaporates at a lower temperature than uranium dioxide (UO 2 ). Therefore, in a TIMS experiment with a sample containing these two compounds, the plutonium signal will appear before that of uranium.…”

Section: Introductionmentioning

confidence: 99%

Determination of the Concentration and Isotope Ratio of Uranium in Soil and Water by Thermal Ionization Mass Spectrometry

Park¹,

Park²,

Song³

2014

Mass Spectrometry Letters

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Thermal ionization mass spectrometry (TIMS) was used to determine the concentration and isotope ratio of uranium contained in samples of soil and groundwater collected from Korea. Quantification of uranium in ground water samples was performed by isotope dilution mass spectrometry. A series of chemical treatment processes, including chemical separation using extraction chromatography, was applied to the soil samples to extract the uranium. No treatments other than filtration were applied to the groundwater samples. Isotopic analyses by TIMS showed that the isotope ratios of uranium in both the soil and water samples were indistinguishable from those of naturally abundant uranium. The concentration of uranium in the groundwater samples was within the U.S. acceptable standards for drinking water. These results demonstrate the utility of TIMS for monitoring uranium in environmental samples with high analytical reliability.

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Simultaneous determination of plutonium and uranium isotope ratios in individual plutonium–uranium mixed particles by thermal ionization mass spectrometry

Cited by 25 publications

References 16 publications

Ambient aging of rhenium filaments used in thermal ionization mass spectrometry: Growth of oxo-rhenium crystallites and anti-aging strategies

Ambient aging of rhenium filaments used in thermal ionization mass spectrometry: Growth of oxo-rhenium crystallites and anti-aging strategies

Direct isotope ratio analysis of individual uranium–plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry

Determination of the Concentration and Isotope Ratio of Uranium in Soil and Water by Thermal Ionization Mass Spectrometry

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