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Journal Articles

Radioactive certified reference materials

Watanabe, Kazuo

Bunseki, 2010(7), p.349 - 350, 2010/07

Outline of radioactive certified reference materials (CRM) for the analysis of nuclear materials and radioactive nuclides were described. The nuclear fuel CRMs are supplied by the three institutes: NBL in the US, CETAMA in France and IRMM in Belgium. For the RI CRMs, the Japan Radioisotope Association is engaged in activities concerning supply. The natural-matrix CRMs for the analysis of trace levels of radio-nuclides are prepared and supplied by NIST in the US and the IAEA.

Journal Articles

Ablation-initiated isotope-selective atomic absorption spectroscopy of lanthanide elements

Miyabe, Masabumi; Oba, Masaki; Iimura, Hideki; Akaoka, Katsuaki; Maruyama, Yoichiro; Wakaida, Ikuo; Watanabe, Kazuo

AIP Conference Proceedings 1104, p.30 - 35, 2009/03

no abstracts in English

JAEA Reports

Recent progress of analytical methods of spent nuclear fuel, Review

Yoshida, Zenko; Watanabe, Kazuo; Ito, Mitsuo; Ueno, Takashi; Takeshita, Hidefumi

JAEA-Review 2008-062, 34 Pages, 2009/01

JAEA-Review-2008-062.pdf:4.07MB

Analytical methods for the spent nuclear fuel (SF) have been greatly innovated recently. This methodological innovation is mainly caused by rapid and remarkable progress of induced coupled plasma-mass spectrometry (ICP-MS) which is utilized for the isotopic analysis of actinoid elements (U, Np, Pu, Am, Cm) and fission product elements in the SF samples. The quantity of the objective element as well as the volume of the sample solution needed for the ICP-MS measurement are, in principle, much less than those required for the measurement by other analytical methods. ICP-MS makes it possible to reduce the radiation dose of the operator and to minimize the amount of the radioactive wastes generated from the analytical work. For the precise and accurate isotopic analysis of the objective element in the SF sample by mass spectrometry, the interfering element having isobars needs to be separated prior to the measurement. This review highlights the development of the separation methods and isotopic analysis methods for the analysis of the SF based on more than 50 recent publications and the future problems to be solved and prospects are discussed.

Journal Articles

Dependence of the precision of uranium isotope ratio on particle diameter in individual particle analysis with SIMS

Esaka, Fumitaka; Watanabe, Kazuo; Onodera, Takashi; Lee, C. G.; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu

Applied Surface Science, 255(4), p.1512 - 1515, 2008/12

 Times Cited Count:9 Percentile:40.55(Chemistry, Physical)

Isotope ratio analysis of individual uranium particles in environmental samples taken at nuclear facilities is one of the key techniques for nuclear safeguards. For accurate analysis, we developed a combined technique of single particle manipulation, which was carried out in scanning electron microscope (SEM), and SIMS. This technique gives information on particle size as well as isotope ratios for each particle. In the present study, the particle size dependence of the precision of uranium isotope ratio is investigated by using the SEM-SIMS technique. In the analysis of individual particles of a CRM U050 (5% enriched uranium) sample, even if the particle diameter was 0.5 $$mu$$m, the analysis with the precision of $$^{235}$$U/$$^{238}$$U isotope ratio within 5% was possible. In the presentation, the results obtained for the other uranium particles having different isotopic composition will also be presented.

JAEA Reports

Resonance absorption spectroscopy for laser-ablated lanthanide atom, 1; Optimized experimental conditions for isotope-selective absorption of gadolinium (Contract research)

Miyabe, Masabumi; Oba, Masaki; Iimura, Hideki; Akaoka, Katsuaki; Maruyama, Yoichiro; Wakaida, Ikuo; Watanabe, Kazuo

JAEA-Research 2008-056, 24 Pages, 2008/06

JAEA-Research-2008-056.pdf:5.1MB

For remote isotope analysis of low-decontaminated TRU fuel, we are developing an analytical technique on the basis of the resonance absorption spectroscopy for the laser-ablation plume. To improve isotopic selectivity and detection sensitivity of this technique, we measured absorption spectra of Gd atom with various conditions. As a result, high resolution spectrum was obtained from the observation of slow component of the plume produced under low-pressure rare-gas ambient. The observed narrowest linewidth of about 0.85 GHz was found to be close to the Doppler width estimated for Gd atom of room temperature. Furthermore, relaxation rate of higher meta-stable state was found to be faster than that of ground state, suggesting that use of the transition arising from ground state or lower meta-stable state is preferable for highly sensitive isotope analysis.

Journal Articles

Impregnation of a neutral extractant to hydrophobic/hydrophilic groups introduced into the polymer chain grafted onto a porous membrane

Sawaki, Kenta*; Asai, Shiho; Watanabe, Kazuo; Sugo, Takanobu*; Saito, Kyoichi*

Maku, 33(1), p.32 - 38, 2008/01

TOPO, tri-n-octylphosphine oxide, as a neutral extractant was impregnated to the hydrophobic group of the polymer chain grafted onto a porous hollow-fiber membrane for an efficient metal-ion collection. A diol group,i.e., adjacent hydroxyl group was introduced into poly-glycidyl methacrylate(GMA) chain grafted onto the porous hollow-fiber membrane via the epoxy-ring-opening reaction with water, followed by a reaction of the remaining epoxy group with octadecanethiol (C$$_{18}$$H$$_{37}$$SH) to form an octadecanethiol group. The diol group reduced the amount of TOPO coagulatedon the graft chain, whereas the interaction of the octadecanethiol group of the graft chain with the hydrophobic part of TOPO enabled the impregnation of TOPO to the graft chain. A 1 mmol-Bi/L bismuth chloride solution was forced to permeate through the pores of the TOPO-impregnated porous hollow-fiber membrane with a density of TOPO impregnated of 1.3 mol/kg of the GMA-grafted porous hollow-fiber membrane and the pure water flux of 0.7 m/h at 0.1 MPa and 298 K. The equilibrium binding capacity of the membrane for bismuth ions was 0.22 mol/kg of the TOPO-impregnated porous hollow-fiber membrane, which was equivalent to a binding ratio of bismuth ion to impregnated TOPO of 1.0.

Journal Articles

Application of Inductively coupled plasma Mass Spectrometry to the determination of uranium isotope ratios in individual particles for nuclear safeguards

Zhang, X. Z.*; Esaka, Fumitaka; Esaka, Konomi; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu; Watanabe, Kazuo

Spectrochimica Acta, Part B, 62(10), p.1130 - 1134, 2007/10

 Times Cited Count:23 Percentile:70.33(Spectroscopy)

The capability of inductively coupled plasma mass spectrometry (ICP-MS) for the determination of uranium isotope ratios in individual particles was determined. For this purpose, we developed an experimental procedure including single particle transfer with a manipulator, chemical dissolution and isotope ratio analysis. As the result, the $$^{235}$$U/$$^{238}$$U isotope ratio for the particle with the diameter between 0.5 and 3.9 $$mu$$m was successfully determined with the deviation from the certified ratio within 1.8%. The developed procedure was successfully applied to the analysis of a simulated environmental sample prepared from a mixture of indoor dust (NIST SRM 2583) and uranium particles (NBL CRM U050, U350 and U950a). From the results, the proposed procedure was found to be an alternative analytical tool for nuclear safeguards.

Journal Articles

Development in fission track- thermal ionization mass spectrometry for particle analysis of safeguards environmental samples

Lee, C. G.; Iguchi, Kazunari; Inagawa, Jun; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki; Sakurai, Satoshi; Watanabe, Kazuo; Usuda, Shigekazu

Journal of Radioanalytical and Nuclear Chemistry, 272(2), p.299 - 302, 2007/05

 Times Cited Count:47 Percentile:93.88(Chemistry, Analytical)

no abstracts in English

Journal Articles

Journal Articles

Impregnation of an acidic extractant cyanex 272 to the alkylamino group and alkylthiol group introduced into the polymer chain grafted onto a porous membrane

Sawaki, Kenta*; Domon, Sayaka*; Asai, Shiho; Watanabe, Kazuo; Sugo, Takanobu*; Saito, Kyoichi*

Maku, 32(2), p.109 - 115, 2007/03

no abstracts in English

Journal Articles

Particle isolation for analysis of uranium minor isotopes in individual particles by secondary ion mass spectrometry

Esaka, Fumitaka; Esaka, Konomi; Lee, C. G.; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu; Watanabe, Kazuo

Talanta, 71(3), p.1011 - 1015, 2007/02

 Times Cited Count:63 Percentile:87.33(Chemistry, Analytical)

A new technique to measure $$^{234}$$U/$$^{238}$$U and $$^{236}$$U/$$^{238}$$U isotope ratios for individual particles in safeguards environmental samples was developed, which was a combination of particle isolation under scanning electron microscope (SEM) and secondary ion mass spectrometry (SIMS). In order to verify the effectiveness of the technique, the $$^{234}$$U/$$^{238}$$U and $$^{236}$$U/$$^{238}$$U isotope ratios were measured for individual particles in a simulated environmental sample containing uranium standard (NIST CRM U010) and Pb metal particles. The deviations of the $$^{234}$$U/$$^{238}$$U and $$^{236}$$U/$$^{238}$$U isotope ratios from the certified values increased with increasing the signal intensity ratio of $$^{208}$$Pb to $$^{238}$$U, which was due to the interferences by Pb molecular ions. By the isolation of individual uranium particles prior to SIMS analysis, the interferences were eliminated. The effectiveness of the technique was also confirmed by the analysis of a real sample taken at a laboratory in Japan Atomic Energy Agency (JAEA).

Journal Articles

Preparation of Aliquat 336-impregnated porous membrane

Asai, Shiho; Watanabe, Kazuo; Saito, Kyoichi*; Sugo, Takanobu*

Journal of Membrane Science, 281(1-2), p.195 - 202, 2006/09

 Times Cited Count:13 Percentile:44.25(Engineering, Chemical)

Aliquat 336, tri-${it n}$-octylmethylammonium chloride, was impregnated into the polymer chain grafted onto a porous membrane. 6-aminohexanoic acid and octadecylamine were introduced into the epoxy group of the graft chain. The amount of impregnated Aliquat 336 was 1.2 mol per kg of the GMA-grafted porous membrane. The coexistence of 6-aminohexanoic acid and octadecylamino groups enabled the high-density and stable impregnation of Aliquat 336 to the graft chain. Palladium chloride dissolved in 1 M hydrochloric acid was forced to permeate through the pores of the Aliquat 336-impregnated porous membrane. The binding efficiency was found to be 69%.

Journal Articles

Single particle transfer for quantitative analysis with total-reflection X-ray fluorescence spectrometry

Esaka, Fumitaka; Esaka, Konomi; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu; Watanabe, Kazuo

Nuclear Instruments and Methods in Physics Research B, 251(1), p.218 - 222, 2006/09

 Times Cited Count:3 Percentile:21.09(Instruments & Instrumentation)

Individual Cu particles were transferred, with a manipulator attached to a scanning electron microscope, onto individual Si carriers for subsequent quantitative analysis by means of total-reflection X-ray fluorescence spectrometry. By applying an internal standard to the carriers prior to the particle transfer, the amounts of Cu were successfully determined for the particles with diameters between 3.04 and 8.84 micrometer. The deviations of the measured values from the calculated ones were within 10%. However, the deviations were more than 33% if particle diameters were greater than 10.17 micrometer. This suggests that in such a case the fluorescent X-ray is not emitted from all parts of the particle. Even if particle diameters were greater than 10.17 micrometer, the amounts of Cu could be determined with the deviations within 9% when the particles were dissolved with HNO$$_{3}$$ solution. This technique was also successfully applied to the measurement of individual brass particles.

Journal Articles

Challenge to ultra-trace analytical techniques of nuclear materials in environmental samples for safeguards at JAERI; Methodologies for physical and chemical form estimation

Usuda, Shigekazu; Yasuda, Kenichiro; Kokubu, Yoko; Esaka, Fumitaka; Lee, C. G.; Magara, Masaaki; Sakurai, Satoshi; Watanabe, Kazuo; Hirayama, Fumio; Fukuyama, Hiroyasu; et al.

International Journal of Environmental Analytical Chemistry, 86(9), p.663 - 675, 2006/08

 Times Cited Count:14 Percentile:40.18(Chemistry, Analytical)

The IAEA introduced the environmental sample analysis method, as a powerful tool to detect undeclared nuclear activities, into strengthened safeguards system. The principle of the method is that nuclear signatures can be evidenced if trace amount of nuclear materials in environmental samples taken from inside and outside of nuclear facilities are accurately analyzed. Currently, isotope ratios of uranium and plutonium in "swipe" samples are measured, which are collected in nuclear facilities. In future, the subject of environmental sample analysis will expand to soil, sediment, vegetation, water and airborne dust taken from outside of the nuclear facilities. If physical and chemical form of the nuclear materials is identified, we may estimate their origin, treatment process and migration behavior. This paper deals with the developed analytical techniques for the safeguards environmental samples, the current R&D on techniques related to estimation of the physical and chemical form, and possible analytical methodologies applicable to ultra-trace amounts of nuclear materials.

Journal Articles

Development of frequency stabilized diode laser based on a spectroscopic study on magnetically induced circular dichroism of atomic rubidium

Miyabe, Masabumi; Kato, Masaaki; Oba, Masaki; Wakaida, Ikuo; Watanabe, Kazuo; Wendt, K.*

Japanese Journal of Applied Physics, Part 1, 45(5A), p.4120 - 4122, 2006/05

 Times Cited Count:2 Percentile:8.72(Physics, Applied)

We developed a frequency-stabilized diode laser using magnetically induced circular dichroism. From a spectroscopic study on Rb-${it D}$ $$_{2}$$ line, the most stable Doppler-broadened and Doppler-free lines were determined to be the transition from ${it F}$g=2 ground state of $$^{85}$$Rb and the crossover resonance from ${it F}$g=3 ground state to ${it F}$e=3 and 4 excited states of $$^{85}$$Rb respectively. Furthermore, we measured the fluctuation of the laser locked to the Doppler-free line to be $$pm$$50kHz/8hour and thus revealed the applicability to a several-hours stabilization. The developed laser can be used as a reference laser for frequency stabilization system for multiple tunable lasers for RIMS analysis.

Journal Articles

Development of RIMS apparatus for isotope analysis of Calcium nuclear waste materials

Miyabe, Masabumi; Oba, Masaki; Kato, Masaaki; Wakaida, Ikuo; Watanabe, Kazuo

Journal of Nuclear Science and Technology, 43(4), p.305 - 310, 2006/04

 Times Cited Count:13 Percentile:65.83(Nuclear Science & Technology)

We are developing an resonance ionization spectrometric apparatus aiming at an analysis of a radioactive isotope of calcium ($$^{41}$$Ca) in nuclear waste materials. The developed system consists of the reference laser whose frequency was locked on a Doppler-free absorption line of 85Rb and the computer-controlled fringe offset lock system which transfer frequency stability of the reference laser to slave lasers for Ca excitation. With heterodyne spectroscopy and laser induced fluorescence spectroscopy of Ca, it was confirmed that the developed apparatus was suitable for resonance ionization spectrometric analysis.

Journal Articles

Influence of uranium enrichment on the etching rate of polycarbonate fission track detector containing uranium particles

Lee, C. G.; Iguchi, Kazunari; Esaka, Fumitaka; Magara, Masaaki; Sakurai, Satoshi; Watanabe, Kazuo; Usuda, Shigekazu

Nuclear Instruments and Methods in Physics Research B, 245(2), p.440 - 444, 2006/04

 Times Cited Count:8 Percentile:50.31(Instruments & Instrumentation)

The etching rates of fission track detectors made of polycarbonate containing uranium particles were measured after thermal neutron irradiation with fluence of 8$$times$$10$$^{14}$$ n/cm$$^{2}$$, in order to study the influence of uranium enrichment on the etching rate that was calculated from the weight loss by etching. There is a strong correlation between the etching rate of detector and the enrichment E of uranium particle: the former increases as the latter increases. Particularly, the etching rate per particle was proportional to E$$^{2/3}$$ rather than E$$^{1}$$, which is probably due to the overlapping of fission tracks. The etching behaviors of detector revealed that the existence of two different etching rate regions, a nonlinear region in the beginning of etching process and a subsequent constant region, which was explained as the opening of fission tracks and the broadening of opened tracks, respectively.

Journal Articles

Improved method of fission track sample preparation for detecting particles containing fissile materials in safeguards environmental samples

Lee, C. G.; Iguchi, Kazunari; Esaka, Fumitaka; Magara, Masaaki; Sakurai, Satoshi; Watanabe, Kazuo; Usuda, Shigekazu

Japanese Journal of Applied Physics, Part 2, 45(10), p.L294 - L296, 2006/03

 Times Cited Count:18 Percentile:54.95(Physics, Applied)

We have developed an effective method for fission track (FT) sample preparation to perform particle analysis of the safeguards environmental samples by the FT-thermal ionization mass spectrometry (TIMS) method. In this method, a fission track detector and the layer containing particles are separated. The main feature of the developed FT sample is that the detection of a particle from the corresponding fission track can be performed correctly and in a simple manner by fixing each one end of the detector and the particle layer and by using an etching tool. It is expected that this method will enhance the effectiveness of particle analysis.

Journal Articles

Determination of ionization potential of calcium by high-resolution resonance ionization spectroscopy

Miyabe, Masabumi; Geppert, C.*; Kato, Masaaki; Oba, Masaki; Wakaida, Ikuo; Watanabe, Kazuo; Wendt, K. D. A.*

Journal of the Physical Society of Japan, 75(3), p.034302_1 - 034302_10, 2006/03

 Times Cited Count:18 Percentile:65.97(Physics, Multidisciplinary)

High-resolution resonance ionization spectroscopy has been utilized to determine a precise ionization potential of Ca. Three-step resonance excitation with single-mode extended cavity diode lasers populates long and unperturbed Rydberg series of 4snp (1P1) and 4snf (1F3) states in the rage of n=20-150. By using an extended Ritz formula for quantum defect, the series convergence limit has been determined to be 49305.9240 (20) cm$$^{-1}$$ with the accuracy improved one order of magnitude higher than previously reported ones.

Journal Articles

Development of analytical techniques for safeguards environmental samples at JAEA

Sakurai, Satoshi; Magara, Masaaki; Usuda, Shigekazu; Watanabe, Kazuo; Esaka, Fumitaka; Hirayama, Fumio; Lee, C. G.; Yasuda, Kenichiro; Inagawa, Jun; Suzuki, Daisuke; et al.

Kaku Busshitsu Kanri Gakkai (INMM) Nihon Shibu Dai-27-Kai Nenji Taikai Rombunshu (CD-ROM), 9 Pages, 2006/00

no abstracts in English

105 (Records 1-20 displayed on this page)