• Mass Spectrometry Letters
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• v.5 no.1
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• pp.12-15
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• 2014

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.

• Economic and Environmental Geology
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• v.56 no.5
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• pp.547-555
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• 2023

Due to enhanced precision in uranium isotope measurements with MC-ICP-MS, there has been a surge in studies concerning the naturally occurring uranium isotope ratio (²³⁸U/²³⁵U) and its associated fractionation processes. Several researchers have highlighted that the ²³⁸U/²³⁵U ratio, previously assumed to be constant, can vary by several per mil depending on different natural fractionation processes. This review paper outlines the uranium isotope values (δ²³⁸U) for major terrestrial reservoirs and their variations. It discusses the range of δ238U values and uranium isotope fractionation seen in uranium ore deposits, based on deposit type and ore-forming conditions. In conclusion, this paper emphasizes the importance of studies on uranium ore deposits. Such deposits serve as natural simulation models vital for designing high-level radioactive waste repository sites.

• Mass Spectrometry Letters
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• v.2 no.4
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• pp.80-83
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• 2011

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.

• Mass Spectrometry Letters
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• v.1 no.1
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• pp.17-20
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• 2010

As background significantly affects measurement accuracy and a detection limit in determination of the trace amounts of uranium, it is necessary to minimize the impurities in the filaments used for thermal ionization mass spectrometry (TIMS). We have varied the degassing condition such as the heating currents and duration times to reduce the backgrounds from the filaments prepared with zone-refined rhenium tape. The most efficient degassing condition of the heating current and the duration time was determined as 3.5 A and 60 min, respectively. The TIMS measurement combined with the isotope dilution mass spectrometry (IDMS) technique showed that the uranium backgrounds were determined to be in a few fg level from blank rhenium filaments. The background minimized filaments were utilized to measure the uranium isotope ratios of a U030 (NIST) standard sample. The excellent agreement of the measurement with the certified isotope ratios showed that the degassing procedure optimized in this study efficiently reduced the impurity signals of uranium from blank rhenium filaments to a negligible level.

• Nuclear Engineering and Technology
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• v.29 no.4
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• pp.327-335
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• 1997

The correlation of isotope composition of uranium, plutonium and neodymium with the burnup in M uranium dioxide fuel has been investigated experimentally. The total and fractional($^{235}$ U) burnup were determined by Nd-148 and, U and Pu mass spectrometric method respectively. The isotope compositions of these elements, after their separation from the fuel samples were measured by mass spectrometric. The content of the elements in the irradiated fuel ore determined by isotope dilution mass spectrometric method using $^{233}$ U, $^{242}$ Pu and $^{150}$ Nd as spikes. The content of plutonium in the irradiated fuel was expressed by the correlation with uranium isotopes. The correlations between isotope compositions themselves and the total and fractional burnup ore compared with those calculated from ORIGEN2 code.

• Mass Spectrometry Letters
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• v.7 no.2
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• pp.41-44
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• 2016

Secondary ion mass spectrometry (SIMS) is a promising tool to measure isotope ratios of individual uranium particles in environmental samples for nuclear safeguards. However, the analysis requires prior identification of a small number of uranium particles that coexist with a large number of other particles without uranium. In the present study, this identification was performed by scanning electron microscopy - energy dispersive X-ray analysis with automated particle search mode. The analytical results for an environmental sample taken at a nuclear facility indicated that the observation of backscattered electron images with × 1000 magnification was appropriate to efficiently identify uranium particles. Lower magnification (less than × 500) made it difficult to detect smaller particles of approximately 1 μm diameter. After identification, each particle was manipulated and transferred for subsequent isotope ratio analysis by SIMS. Consequently, the isotope ratios of individual uranium particles were successfully determined without any molecular ion interference. It was demonstrated that the proposed technique provides a powerful tool to measure individual particles not only for nuclear safeguards but also for environmental sciences.

• Nuclear Engineering and Technology
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• v.52 no.7
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• pp.1532-1536
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• 2020

For ensuring nuclear safeguards, we report the analytical signal-detection performance of thermal ionization mass spectrometry (TIMS) with continuous heating for the measurement of isotopic ratios in samples containing ultra-trace amounts of uranium. As methods for detecting uranium signals, peak-jumping mode using a single detector and static mode using multiple detectors were examined with U100 (10% ²³⁵U-enriched) uranium standard samples in the femtogram-to-picogram range. Uranium isotope ratios, n(²³⁵U)/n(²³⁸U), were measured down to levels of 1 fg and 3 fg in static and peak-jumping modes, respectively, while n(²³⁴U)/n(²³⁸U) and n(²³⁶U)/n(²³⁸U) values were measured down to levels of 100 fg in both modes. In addition, the dependency of the ²³⁸U signal intensity on sample quantity exhibited similar tendencies in both modes. The precisions of the isotope ratios obtained in the static mode over all sample ranges used in this study were overall slightly higher than those obtained in peak-jumping mode. These results indicate that isotope ratio measurements by TIMS with continuous heating are almost independent of the detection method, i.e., peak-jumping mode or static mode, which is characteristic of isotope-ratio measurements using the TIMS method with continuous heating. TIMS with continuous heating is advantageous as it exhibits the properties of multiple detectors within a single detector, and is expected to be used in various fields in addition to ensuring nuclear safeguards.

• Mass Spectrometry Letters
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• v.3 no.2
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• pp.54-57
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• 2012

Mass spectrometric analysis was carried out using multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS) for the precise and accurate determination of the isotope ratios of ultratrace levels of uranium dissolved in 3% $HNO_3$. We used the certified reference material (CRM) 112-A at a trace level of 100 pg/mL for the uranium isotopic measurement. Multiple collectors were utilized for the simultaneous measurement of uranium isotopes to reduce the signal uncertainty due to variations in the ion beam intensity over time. Mass bias correction was applied to the measured U isotopes to improve the precision and accuracy. Furthermore, elemental standard solution with certified values of platinum, iridium, gold, and thallium dissolved in 3% $HNO_3$ were analyzed to investigate the formation rates of the polyatomic ions of $Ir^{40}$ $Ar^+$, $Pt^{40}$ $Ar^+$, $Tl^{40}$ $Ar^+$, $Au^{40}$ $Ar^+$ for the concentration range of 50-400 pg/mL. Those polyatomic ions have mass-to-charge ratios in the 230-245 m/z region that it would contribute to the increase of background intensity of uranium, thorium, plutonium, and americium isotopes. The effect of the polyatomic ion interference on uranium isotope measurement has been estimated.

• Mass Spectrometry Letters
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• v.7 no.3
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• pp.64-68
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• 2016

Scanning electron microscopy combined with thermal ionization mass spectrometry (SEM-TIMS) was used to determine the precise isotope ratios of ultra-trace levels of uranium contained in individual microparticles. An advanced multiple ion counter system consisting of three secondary ion multipliers and two compact discrete dynodes was used for complete simultaneous ion detection. For verification purposes, using TIMS with complete simultaneous measurement, isotopes were analyzed in 5 pg of uranium of a certified reference material. A microprobe in the SEM was used to transfer individual particles from a NUSIMEP-7 sample to TIMS filaments, which were then subjected to SEM-TIMS and complete simultaneous measurement. The excellent agreement in the resulting uranium isotope ratios with the certified NUSIMEP-7 values shows the validity of SEM-TIMS with complete simultaneous measurement for the analysis of uranium isotopes in individual particles. Further experimental study required for investigation of simultaneous measurement using the advanced multiple ion counter system is presented.

• Nuclear Engineering and Technology
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• v.52 no.12
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• pp.2867-2873
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• 2020

In reprocessed uranium, derived from an impoverished fuel of light-water moderated reactors, there are isotopes of ^{232, 234, 236}U, which make its recycling remarkably difficult. A method of concentration of ²³⁵U target isotope in cascade's additional product was proposed to recover the isotopic composition of reprocessed uranium. A general calculation procedure is presented and a parameters' optimization of multi-flow cascades with additional products. For the first time a numeric model of a cascade that uses the cuts of partial flows of stages with relatively high separation factors was applied in this procedure. A novel computing experiment is carried out on separation of reprocessed uranium hexafluoride with providing a high concentration of ²³⁵U in cascade's additional product with subsequent dilution. The parameters of cascades' stages are determined so as to allow reducing the ^{232, 234, 236}U isotope content up to the acceptable. It was demonstrated that the dilution of selected products by the natural waste makes it possible to receive a low enriched uranium hexafluoride that meets the ASTM C996-15 specification for commercial grade.