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U/
U isotopic analysis of trace uranium in safeguards environmental samples using multicollector inductively coupled plasma mass spectrometryTomita, Jumpei; Tomita, Ryohei; Suzuki, Daisuke; Yasuda, Kenichiro; Miyamoto, Yutaka
Journal of the American Society for Mass Spectrometry, 35, p.1178 - 1183, 2024/05
A sensitive analytical technique was investigated in order to determine 10
order of U/U ratio in the sub-ng of uranium using a multi-collector ICP-MS. First, the solution volume was concentrated to one tenth to obtain higher intensities. Next, data acquisition was started from the beginning of the solution uptake and continued until all solution was exhausted. Taking advantage of multi-collector measurement, all data were used with excepting the portion affected by air mixing at the beginning and end of sample introduction. The isotope ratios were calculated from the total counts of each isotope. This technique was applied to U isotope standard (IRMM-184) to measure the 10 order of U/U ratio in the sub-ng of uranium. Measured values were in good agreement with the certified value within the uncertainity (
=2). The uncertainties obtained with this new technique (32% on average) were revised to be 10 times smaller than those obtained with the conventionalmethod.
NiShizuma, Toshiyuki*; Omer, M.; Hayakawa, Takehito*; Minato, Futoshi*; Matsuba, Shunya*; Miyamoto, Shuji*; Shimizu, Noritaka*; Utsuno, Yutaka
Physical Review C, 109(1), p.014302_1 - 014302_7, 2024/01
Times Cited Count：0 Percentile：0.11(Physics, Nuclear)
CUtsunomiya, Hiroaki*; Goriely, S.*; Kimura, Masaaki*; Shimizu, Noritaka*; Utsuno, Yutaka; Tveten, G. M.*; Renstr
m, T.*; Ariizumi, Takashi*; Miyamoto, Shuji*
Physical Review C, 109(1), p.014617_1 - 014617_7, 2024/01
Times Cited Count：0 Percentile：0.11no abstracts in English
Tomita, Ryohei; Tomita, Jumpei; Suzuki, Daisuke; Yasuda, Kenichiro; Miyamoto, Yutaka
Hosha Kagaku, (48), p.1 - 15, 2023/09
Secondary Ion Mass Spectrometry (SIMS) is the method to detect secondary ions produced by the sputtering of primary ions. SIMS is one of effective method to measure isotopic composition of particles containing nuclear material in environmental sample for safeguards. We are a group member of the International Atomic Energy Agency (IAEA)'s network of analytical laboratories and have developed analytical techniques using SIMS and other mass spectrometers for nuclear safeguards. We will introduce the principle of SIMS and analytical techniques developed by our group to measure isotopic composition of uranium particles which having a particle diameter of micron order in environmental sample for safeguards.
Miyamoto, Yutaka; Suzuki, Daisuke; Tomita, Ryohei; Tomita, Jumpei; Yasuda, Kenichiro
Isotope News, (786), p.22 - 25, 2023/04
no abstracts in English
Tomita, Jumpei; Tomita, Ryohei; Suzuki, Daisuke; Yasuda, Kenichiro; Miyamoto, Yutaka
KEK Proceedings 2022-2, p.154 - 158, 2022/11
Precise determination of minor U isotopes (
U and U) of particles from the safeguard environmental samples is powerful method for detecting the undeclared nuclear activities. In this study, preparation method of U particle was examined to utilize for the minor U isotope determination. The porous silica particles were used as the particle matrix and lutetium was mixed to the impregnation solution as U impregnation indicator for the particle picking. The result of the Scanning Electron Microscope indicated that the contacting the solution with Si particles overnight gently could produce the impregnated particles effectively rather than the mixing them with PFA stick.
Yomogida, Takumi; Kitatsuji, Yoshihiro; Miyamoto, Yutaka
KEK Proceedings 2022-2, p.148 - 153, 2022/11
The Research Group for Safeguards Analytical Chemistry is currently developing a method to analyze the chemical state of uranium particles in environmental samples collected at nuclear facilities using micro-Raman spectroscopy. The chemical state of uranium particles in environmental samples can be partially oxidized by long-term exposure to air. It is necessary to develop a method to analyze the chemical state of the entire particle. In this study, uranium dioxide stored under atmospheric conditions was analyzed by micro-Raman mapping. The Raman spectra showed that uranium peroxide was locally present in the UO
particle. The Raman peaks originating from the structure of UO around 570 cm
and 1150 cm could not be observed in the point analysis of the particle center. On the other hand, in mapping analysis, Raman peaks originating from the structure of UO can be observed from the same particle, demonstrating that Raman mapping analysis is an effective method for analyzing the chemical state of the entire particle.
Tomita, Ryohei; Tomita, Jumpei; Yomogida, Takumi; Suzuki, Daisuke; Yasuda, Kenichiro; Esaka, Fumitaka; Miyamoto, Yutaka
KEK Proceedings 2022-2, p.108 - 113, 2022/11
Automated Particle Measurement (APM) is the first measurement of environmental sample for safeguard purpose. APM tells us the number of particles in sample, their enrichment and their location. Precision and accuracy of APM is easily affected by particle condition. We have investigated how influential baking temperature in sample preparation are for uranium secondary ion quantity, uranium hydride generation and particle crystallinity. Our experimental results showed that baking temperature of 800
C reduced uranium secondary ion quantity to 33% compared with baking at 350C. Uranium hydride generation ratio of the sample baked at 850C was also 4 times higher than the sample baked at 350C. Baking at 850C raised only crystallinity of uranium particles. Baking sample at too high temperature caused less uranium secondary ion generation and much more uranium hydride generation. It made precision and accuracy of APM worse. In our experiment, baking at 350C is suitable for uranium particles in the safeguards sample.
Tomita, Ryohei; Tomita, Jumpei; Yomogida, Takumi; Suzuki, Daisuke; Yasuda, Kenichiro; Esaka, Fumitaka; Miyamoto, Yutaka
KEK Proceedings 2021-2, p.146 - 150, 2021/12
no abstracts in English
Ra in natural water samples by ICP-MSTomita, Jumpei; Ozawa, Mayumi; Ohara, Yoshiyuki; Miyamoto, Yutaka
KEK Proceedings 2021-2, p.130 - 134, 2021/12
no abstracts in English
Suzuki, Daisuke; Tomita, Ryohei; Tomita, Jumpei; Esaka, Fumitaka; Yasuda, Kenichiro; Miyamoto, Yutaka
Journal of Radioanalytical and Nuclear Chemistry, 328(1), p.103 - 111, 2021/04
Times Cited Count：3 Percentile：43.41(Chemistry, Analytical)An analytical technique was developed to determine the age of uranium particles for safeguards. After the chemical separation of uranium and thorium, the 
Th/
U ratio was measured using single-collector inductively coupled plasma mass spectrometry and a U-based reference material comprising a certain amount of 
Th as a progeny nuclide of U. The results allowed us to determine the purification age of two certified materials, i.e., U-850 and U-100, which was in good agreement with the reference purification age (61 y). Moreover, the age of a single U-850 particle was determined with a difference of -28 to 2 years from the reference date.
Miyamoto, Yutaka; Yasuda, Kenichiro
Journal of Nuclear and Radiochemical Sciences (Internet), 18, p.13 - 15, 2018/07
A sequential separation technique using an anion-exchange column developed in the previous works have the potential to completely separate picograms of Am from the lanthanides using mixtures of acetic acid, hydrochloric acid, and nitric acid as the eluents, without any functional ligands or special columns. This experimental result implies that ultra-trace actinides, including Am, Pu, U, and Th in environmental samples can be sequentially separated by combination of these mixed-media eluents and an anion exchange column.
Miyamoto, Yutaka; Yasuda, Kenichiro; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki
KEK Proceedings 2017-6, p.292 - 298, 2017/11
Our updated analytical techniques of ultra-trace plutonium in the IAEA environmental samples by ICP-MS were mentioned. Some careful techniques to accurately determine ultra-trace plutonium in the range of femto-grams to pico-grams were introduced. The uncertainties of analytical results were estimated according to the GUM concept. Our trials of determination of sub-femto grams americium in an environmental sample were also mentioned.
Pu/
Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MSEsaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki
Talanta, 165, p.122 - 127, 2017/04
Times Cited Count：15 Percentile：51.61(Chemistry, Analytical)The isotope ratios of Pu/Pu, 
Pu/Pu, 
Pu/Pu, and 
Pu/Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the Pu/Pu, Pu/Pu, and Pu/Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of uranium, plutonium and americium with UTEVA resins. Furthermore, Pu/Pu isotope ratios were able to be calculated by using both the Pu/(Pu+Pu) activity ratios that had been measured through alpha spectrometry and the Pu/Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including Pu/Pu, in individual U-Pu mixed oxide particles.
Miyamoto, Yutaka; Yasuda, Kenichiro; Magara, Masaaki
Journal of Radioanalytical and Nuclear Chemistry, 309(1), p.303 - 308, 2016/07
Times Cited Count：2 Percentile：19.46(Chemistry, Analytical)The technique of sequential separation for U, Th, Pb, lanthanides and Pu using a single anion-exchange column and mixed acids media were developed. An automatic system utilizing a small column and pressurized gas was assembled for this sequential separation. By adjusting the eluent chemical composition for Pu separation, this separation technique has been achieved. Some pieces of tree ring sample were digested, and ultra-trace U and Pu in the samples were separated by this system. The analytical results of U and Pu measured by mass spectrometry will be mentioned.
Esaka, Fumitaka; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki
Journal of Radioanalytical and Nuclear Chemistry, 306(2), p.393 - 399, 2015/11
Times Cited Count：6 Percentile：45.29(Chemistry, Analytical)An analytical technique was developed by a combination of single particle dissolution, chemical separation of uranium, plutonium and americium with extraction chromatography using UTEVA resins and measurement with inductively coupled plasma mass spectrometry (ICP-MS). This method was applied to plutonium isotope ratio analysis of individual U-Pu particles with U/Pu ratios ranging from 1 to 70. Consequently, Pu/Pu, Pu/Pu and Pu/Pu isotope ratios were successfully determined, while it was impossible to determine Pu/Pu ratios due to the high process blank values on m/z 238.
Miyamoto, Yutaka; Yasuda, Kenichiro; Magara, Masaaki
KEK Proceedings 2015-4, p.44 - 48, 2015/11
We developed an automatic system for sequential separation with an anion-exchange column to simply and quickly separate less than pico-grams of ultra-trace U, Th, Pb, the lanthanide, and Pu in an environmental sample without foreign contamination. The objective sequential separation of ultra-trace multi-elements succeeded by choosing the HCl-HF mixture based acetic acid for Th separation and the HCl-diluted HF mixture for Pu separation. The objective elements in a multi-elements mixture were completely separated for 6 h 15 min by use of the automatic system and the optimized separation condition.
Miyamoto, Yutaka; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki
Analytical and Bioanalytical Chemistry, 407(23), p.7165 - 7173, 2015/09
Times Cited Count：8 Percentile：31.01(Biochemical Research Methods)Age of individual uranium-plutonium mixed particles with various U/Pu atomic ratios were determined by inductively-coupled plasma mass spectrometry. Micron-sized particles were prepared from U and Pu certified reference materials. The Pu reference was stored for 4-6 years since the last purification. The Pu purification age was obtained from the Am/Pu ratio which was calculated from the product of three measured ratios of Pu and Am isotopes in the eluted fractions. Am, U and Pu in a sample solution were sequentially separated a small anion-exchange column. The Am/Pu ratio was accurately determined by spiking pure 
Am to the sample solution. The determined age of particles with various U/Pu ratios was in good agreement with the expected age with high accuracy and high precision.
Miyamoto, Yutaka; Yasuda, Kenichiro; Magara, Masaaki
Analyst, 140(13), p.4482 - 4488, 2015/07
Times Cited Count：6 Percentile：21.34(Chemistry, Analytical)Uranium, Thorium, lead, and the lanthanides were automatically and sequentially separated with a single anion-exchange column. This separation was achieved using eluents consisting of simple and highly pure acid mixture of HCl, HNO
, acetic acid, and HF. This simple, automatic system is driven with pressurized nitrogen gas, and controlled by a computer program. For an evaluation examination, a reference powdered rock sample was separated by using this system. Abundances of objective elements, including 0.23 ng of lutetium, were accurately determined without corrections of chemical recovery yield or subtraction of processing blank. This separation technique saves time and effort for chemical processing, and it is useful for ultra-trace quantitative and isotopic analyses of elements in small environmental samples.
Suzuki, Daisuke; Esaka, Fumitaka; Miyamoto, Yutaka; Magara, Masaaki
Applied Radiation and Isotopes, 96, p.52 - 56, 2015/02
Times Cited Count：15 Percentile：77.17(Chemistry, Inorganic & Nuclear)Isotope ratios of uranium and plutonium in individual U-Pu mixed particles with various U/Pu ratios were determined by thermal ionization mass spectrometry with a continuous heating method without chemical separation. Prior to the measurements, micron-sized U-Pu mixed particles with U/Pu ratios of 1, 5, 10, 18 and 70 were produced by using certified reference materials CRM U-010 (1%
U enriched, NBL) and SRM 947 (NBS) solutions. As a result of isotope ratio analysis, accurate values for U and Pu ratios, except for Pu/Pu, were successfully determined for the particles with all U/Pu ratios. Although some pre-treatment such as chemical separation would need for accurate determination of Pu/Pu isotope analysis, it was shown that this analytical technique has a potential of powerful tool for nuclear safeguards and forensics.
