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Journal Articles

Trace analysis for nuclear non-proliferation and security

Esaka, Fumitaka

Bunseki, 2018(10), p.408 - 411, 2018/10

Recent development of analytical techniques for identification of particles containing nuclear materials, isotope ratio analysis of uranium and plutonium using mass spectrometry, and age determination is described in this paper. These techniques are successfully applied to the trace analysis for nuclear non-proliferation.

Journal Articles

Anion-exchange separation of americium and the lanthanides using a single column

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.

Journal Articles

Chemical state and isotope ratio analysis of individual uranium particles by a combination of micro-Raman spectroscopy and secondary ion mass spectrometry

Yomogida, Takumi; Esaka, Fumitaka; Magara, Masaaki

Analytical Methods, 9(44), p.6261 - 6266, 2017/11

 Times Cited Count:5 Percentile:43.21(Chemistry, Analytical)

A combination of micro-sampling, micro-Raman spectroscopy (MRS), and secondary ion mass spectrometry (SIMS) was applied to the characterization of individual uranium particles. Reference particles with U$$_{3}$$O$$_{8}$$ (NBL CRM U010) and UO$$_{2}$$ were identified by scanning electron microscopy combined with energy dispersive X-ray detection (SEM-EDX) and transferred onto grassy carbon substrates by micro-sampling. The crystalline phases of the reference particles with diameters ranging from 1 $$mu$$m to 5 $$mu$$m were determined non-destructively by using MRS thanks to the optimization of laser power at the measurement. Isotope ratios were also determined with SIMS after the MRS analysis and were consistent with values in the literature. These results indicate that chemical forms and isotope ratios of individual uranium particles as small as 1 $$mu$$m can be analyzed efficiently by using the proposed method.

Journal Articles

Accurate sensitive analytical technique of ultra-trace plutonium in the IAEA environmental samples

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.

Journal Articles

Inductively coupled plasma-mass spectrometry

Esaka, Fumitaka

Analytical Sciences, 33(10), p.1097 - 1098, 2017/10

 Times Cited Count:2 Percentile:22.41(Chemistry, Analytical)

Inductively coupled plasma-mass spectrometry (ICP-MS) is widely used in various fields such as environmental, geological, and clinical sciences. In this report, recent advances of the ICP-MS analysis and expected applications are described.

Journal Articles

Analysis of plutonium isotope ratios including $$^{238}$$Pu/$$^{239}$$Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS

Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

Talanta, 165, p.122 - 127, 2017/04

 Times Cited Count:10 Percentile:38.06(Chemistry, Analytical)

The isotope ratios of $$^{238}$$Pu/$$^{239}$$Pu, $$^{240}$$Pu/$$^{239}$$Pu, $$^{241}$$Pu/$$^{239}$$Pu, and $$^{242}$$Pu/$$^{239}$$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 $$^{240}$$Pu/$$^{239}$$Pu, $$^{241}$$Pu/$$^{239}$$Pu, and $$^{242}$$Pu/$$^{239}$$Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of uranium, plutonium and americium with UTEVA resins. Furthermore, $$^{238}$$Pu/$$^{239}$$Pu isotope ratios were able to be calculated by using both the $$^{238}$$Pu/( $$^{239}$$Pu+$$^{240}$$Pu) activity ratios that had been measured through alpha spectrometry and the $$^{240}$$Pu/$$^{239}$$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 $$^{238}$$Pu/$$^{239}$$Pu, in individual U-Pu mixed oxide particles.

Journal Articles

Automatic sequential separation with an anion-exchange column for ultra-trace analysis of Pu, U, Th, Pb, and lanthanides in environmental samples

Miyamoto, Yutaka; Yasuda, Kenichiro; Magara, Masaaki

Journal of Radioanalytical and Nuclear Chemistry, 309(1), p.303 - 308, 2016/07

 Times Cited Count:1 Percentile:83.2(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.

Journal Articles

Uranium particle identification with SEM-EDX for isotopic analysis by secondary ion mass spectrometry

Esaka, Fumitaka; Magara, Masaaki

Mass Spectrometry Letters, 7(2), p.41 - 44, 2016/06

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 $$times$$ 1000 magnification was appropriate to efficiently identify uranium particles. Lower magnification (less than $$times$$ 500) made it difficult to detect smaller particles of approximately 1 $$mu$$m diameter.

Journal Articles

Application of automated particle screening for effective analysis of individual uranium particles by thermal ionization mass spectrometry

Esaka, Fumitaka; Suzuki, Daisuke; Yomogida, Takumi; Magara, Masaaki

Analytical Methods, 8(7), p.1543 - 1548, 2016/02

AA2015-0572.pdf:0.66MB

 Times Cited Count:6 Percentile:42.47(Chemistry, Analytical)

The isotope ratio analysis of individual uranium particles in environmental samples taken at nuclear facilities is important to clarify their origins for nuclear safeguards. In the present study, automated particle screening was used to select uranium particles prior to precise isotope ratio analysis by thermal ionization mass spectrometry (TIMS). As a result, molecular ion interferences on the uranium mass region were able to be almost completely avoided in the analysis of real inspection samples using APM-TIMS. Therefore, the performance of APM-TIMS was sufficient for obtaining isotope ratio data of individual particles without molecular ion interferences.

Journal Articles

Determination of plutonium isotope ratios in individual uranium-plutonium mixed particles with inductively coupled plasma mass spectrometry

Esaka, Fumitaka; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

Journal of Radioanalytical and Nuclear Chemistry, 306(2), p.393 - 399, 2015/11

 Times Cited Count:5 Percentile:46.24(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, $$^{240}$$Pu/$$^{239}$$Pu, $$^{241}$$Pu/$$^{239}$$Pu and $$^{242}$$Pu/$$^{239}$$Pu isotope ratios were successfully determined, while it was impossible to determine $$^{238}$$Pu/$$^{239}$$Pu ratios due to the high process blank values on m/z 238.

Journal Articles

Chemical separation of ultra-trace multi-elements in environmental samples

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.

Journal Articles

Accurate purification age determination of individual uranium-plutonium mixed particles

Miyamoto, Yutaka; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki

Analytical and Bioanalytical Chemistry, 407(23), p.7165 - 7173, 2015/09

 Times Cited Count:6 Percentile:65.45(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 $$^{241}$$Am/$$^{241}$$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 $$^{241}$$Am/$$^{241}$$Pu ratio was accurately determined by spiking pure $$^{243}$$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.

Journal Articles

Surface analysis

Esaka, Fumitaka

Ekisupato Oyo Kagaku Sirizu; Kiki Bunseki, p.119 - 135, 2015/09

Bulk analysis has been conventionally used for measuring solid materials. In contrast, surface analysis is extensively used for analyzing chemical compositions and chemical states of solid surface. The surface compositions often differ from those of bulk materials. Recently, doping of impurity elements and deposition of thin films on the surface of the materials are key techniques to fabricate functional materials. Therefore, surface analysis becomes important to characterize such materials. In this paper, the principle and feature of some surface analytical techniques are described.

Journal Articles

Ultra-trace analysis of plutonium by thermal ionization mass spectrometry with a continuous heating technique without chemical separation

Lee, C.-G.*; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki; Song, K.*

Talanta, 141, p.92 - 96, 2015/08

 Times Cited Count:9 Percentile:54.63(Chemistry, Analytical)

Thermal ionization mass spectrometry (TIMS) with a continuous heating technique is known as an effective method for measuring the isotope ratio in trace amounts of uranium. In this study, the analytical performance of thermal ionization mass spectrometry with a continuous heating technique was investigated using a standard plutonium solution (SRM 947). The influence of the heating rate of the evaporation filament on the precision and accuracy of the isotope ratios was examined using a plutonium solution sample at the fg level. Changing the heating rate of the evaporation filament on samples ranging from 0.1 fg to 1000 fg revealed that the influence of the heating rate on the precision and accuracy of the isotope ratios was slight around the heating rate range of 100 to 250 mA/min. All of the isotope ratios of plutonium (SRM 947), $$^{238}$$Pu/$$^{239}$$Pu, $$^{240}$$Pu/$$^{239}$$Pu, $$^{241}$$Pu/$$^{239}$$Pu and $$^{242}$$Pu/$$^{239}$$Pu, were measured down to sample amounts of 70 fg. The ratio of $$^{240}$$Pu/$$^{239}$$Pu was measured down to a sample amount of 0.1 fg, which corresponds to a PuO$$_{2}$$ particle with a diameter of 0.2 $$mu$$m. Moreover, the signals of $$^{239}$$Pu could be detected with a sample amount of 0.03 fg, which corresponds to the detection limit of $$^{239}$$Pu of 0.006 fg as estimated by the 3 $$sigma$$ criterion. $$^{241}$$Pu and $$^{241}$$Am formed by the decay of $$^{241}$$Pu could be discriminated owing to the difference in the evaporation temperature. As a result, $$^{241}$$Pu/$$^{239}$$Pu as well as $$^{240}$$Pu/$$^{239}$$Pu and $$^{242}$$Pu/$$^{239}$$Pu in plutonium samples could be measured by TIMS with a continuous heating technique and without any chemical separation processes.

Journal Articles

Sequential separation of ultra-trace U, Th, Pb, and lanthanides using a simple automatic system

Miyamoto, Yutaka; Yasuda, Kenichiro; Magara, Masaaki

Analyst, 140(13), p.4482 - 4488, 2015/07

 Times Cited Count:4 Percentile:78.77(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$$_3$$, 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.

Journal Articles

Identifying uranium particles using fission tracks and microsampling individual particles for analysis using thermal ionization mass spectrometry

Esaka, Fumitaka; Suzuki, Daisuke; Magara, Masaaki

Analytical Chemistry, 87(5), p.3107 - 3113, 2015/03

 Times Cited Count:9 Percentile:54.63(Chemistry, Analytical)

The analysis of uranium particles in environmental samples taken from nuclear facilities is a useful tool to unveil undeclared nuclear activities related to the production of nuclear weapons. An efficient method to analyze isotope ratios of individual uranium particles is thermal ionization mass spectrometry (TIMS) combined with a fission track technique. A drawback in the fission track-TIMS technique is so-called particle-mixing. Here, some uranium particles are measured as a single particle and an averaged isotope ratio is obtained, which may lead to misunderstanding conclusions for source identification. In the present study, micro-sampling under a scanning electron microscope has been added to the procedure of the fission track-TIMS technique. The analysis of a mixed sample containing uranium particles in SRM 950a and CRM U100 materials indicated that the problem of particle mixing was almost avoidable with the proposed technique.

Journal Articles

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

Suzuki, Daisuke; Esaka, Fumitaka; Miyamoto, Yutaka; Magara, Masaaki

Applied Radiation and Isotopes, 96, p.52 - 56, 2015/02

 Times Cited Count:13 Percentile:14.19(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%$$^{235}$$U enriched, NBL) and SRM 947 (NBS) solutions. As a result of isotope ratio analysis, accurate values for U and Pu ratios, except for $$^{238}$$Pu/$$^{239}$$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 $$^{238}$$Pu/$$^{239}$$Pu isotope analysis, it was shown that this analytical technique has a potential of powerful tool for nuclear safeguards and forensics.

Journal Articles

Plutonium age determination from $$^{240}$$Pu/$$^{236}$$U ratios in individual particles by ICP-MS without prior chemical separation

Esaka, Fumitaka; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

Microchemical Journal, 118, p.69 - 72, 2015/01

 Times Cited Count:6 Percentile:68.19(Chemistry, Analytical)

The determination of the time elapsed since the last purification of plutonium with chemical separation gives important information for monitoring nuclear activities related to reprocessing and nuclear weapon production. Although methods for the analysis of plutonium solutions have been extensively studied, few studies were conducted for the measurement of individual particles. In this work, a simple technique was developed for age determination of individual plutonium particles by a combination of single particle dissolution and measurement by inductively coupled plasma mass spectrometry (ICP-MS) without prior chemical separation. The analytical results of individual plutonium particles having an age of 5.98 y indicated that the use of $$^{240}$$Pu/$$^{236}$$U ratios allowed for the determination of accurate ages, though that of $$^{238}$$Pu/$$^{234}$$U and $$^{239}$$Pu/$$^{235}$$U ratios was not suitable because of the contamination of natural uranium during the process of sample preparation.

Journal Articles

Size distribution of radioactive particles collected at Tokai, Japan 6 days after the nuclear accident

Miyamoto, Yutaka; Yasuda, Kenichiro; Magara, Masaaki

Journal of Environmental Radioactivity, 132, p.1 - 7, 2014/06

 Times Cited Count:23 Percentile:29.04(Environmental Sciences)

Airborne radioactive particles released by the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident in 2011 were collected with a cascade low-pressure impactor at the Japan Atomic Energy Agency (JAEA) in Tokai. Size-fractionated samples were collected twice, in the periods of March 17 - April 1, 2011, and May 9-13, 2011. These size-fractionated samplings were carried out in the earliest days at a short distance from the FDNPPs. Radioactivity of short-lived nuclides (several ten days of half-life) were determined as well as $$^{134}$$Cs and $$^{137}$$Cs. The elemental composition of size-fractionated samples was also measured. In the first collection, the activity median aerodynamic diameter (AMAD) of $$^{rm 129m}$$Te, $$^{134}$$Cs, $$^{136}$$Cs and $$^{137}$$Cs was 1.5-1.6$$mu$$m, while the diameter of $$^{131}$$I was 0.45$$mu$$m.

Journal Articles

Secondary ion mass spectrometry combined with alpha track detection for isotope abundance ratio analysis of individual uranium-bearing particles

Esaka, Fumitaka; Magara, Masaaki

Talanta, 120, p.349 - 354, 2014/03

 Times Cited Count:8 Percentile:62.32(Chemistry, Analytical)

Secondary ion mass spectrometry (SIMS) was used in combination with alpha track detection for the efficient analysis of uranium-bearing particles with higher $$^{235}$$U abundances in environmental samples. A polycarbonate film containing particles was prepared and placed in contact with a CR-39 plastic detector sheet. After exposure, the sheet was etched in NaOH solution and each uranium-bearing particle was identified through observation of the alpha tracks recorded in the sheet. A portion of the film containing each uranium-bearing particle was cut out and put onto a glassy carbon planchet. The films on the planchet were decomposed through plasma ashing for subsequent uranium abundance ratio analysis with SIMS. The alpha track - SIMS analysis for ten uranium-bearing particles in a sample taken from a nuclear facility afforded $$n$$($$^{235}$$U)/$$n$$($$^{238}$$U) abundance ratios in the range 0.0072 to 0.25, which were significantly higher than those obtained by SIMS without alpha track detection.

151 (Records 1-20 displayed on this page)