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Journal Articles

Treatment technology of highly radioactive solid waste generated by experimental tests and sample analysis in reprocessing facilities

Goto, Yuichi; Inada, Satoshi; Kuno, Takehiko; Mori, Eito*

Nippon Hozen Gakkai Dai-16-Kai Gakujutsu Koenkai Yoshishu, p.221 - 224, 2019/07

Test equipment, containers, and analytical wastes, generated by experiments using spent fuel pieces in hot cell of Operation Testing Laboratory and by analysis of highly active liquid wastes in hot analytical cell line of Tokai Reprocessing Plant, are treated as highly radioactive solid wastes. These wastes are stored in specific shielded containers called waste cask and then transport to the storage facility. The treatment of these highly radioactive solid wastes have been carried out for 40 years with upgrading waste taking out system and transportation device. As a results, automation of several procedures have been achieved utilizing conventional equipment, and work efficiency and safety have been improved.

Journal Articles

Spectrochemistry of technetium by liquid electrode plasma optical emission spectrometry and its applicability of quantification for highly active liquid waste

Yamamoto, Masahiko; Do, V. K.; Taguchi, Shigeo; Kuno, Takehiko; Takamura, Yuzuru*

Spectrochimica Acta, Part B, 155, p.134 - 140, 2019/05

The emission spectra of technetium (Tc) by liquid electrode plasma optical emission spectrometry have been investigated in this study. From the spectra, 52 emission peaks of Tc were observed in the 250-500 nm wavelength range. All peaks were assigned to the neutral state or singly ionized state. The relative intensities of these peaks were similar to those excited by an electric spark. The strongest intensity peaks were found at 254.3 nm, 261.0 nm, and 264.7 nm. Spectral interferences of coexisting elements in highly active liquid waste of reprocessing stream on those three strongest peaks were investigated using simulated sample. No spectral interferences were observed around the 264.7 nm Tc peak. Therefore, analytical performance using 264.7 nm peak was evaluated. The detection limit, estimated on standard and blank samples in 0.4 M nitric acid, was 1.9 mg/L. The relative standard deviation of Tc standard sample (12.0 mg/L) was 3.8% (N = 5, 1$$sigma$$).

Journal Articles

Effect of surface conditions of the filament used in thermal ionization mass spectrometry on an uranium isotopic measurement

Taguchi, Shigeo; Miyauchi, Hironari*; Horigome, Kazushi; Yamamoto, Masahiko; Kuno, Takehiko

Bunseki Kagaku, 67(11), p.681 - 686, 2018/11

In thermal ionization mass spectrometry, de-gassing is one of the important treatments to release impurities of filaments and to minimize the influence of background. In this work, the effect of the surface change in the tungsten filament induced by the conductively heating treatment on uranium isotopic ($$^{235}$$U/$$^{238}$$U) measurement has been investigated. It was found that the conductively heating treatment of the filament has the effect of smoothing the surface of the filament and also has the effect of improving the deposition of the sample on the filament surface. As a result of either these effects, the precision of uranium isotopic ($$^{235}$$U/$$^{238}$$U) measurement was improved.

Journal Articles

Separation technique using column chromatography for safeguards verification analysis of uranium and plutonium in highly-active liquid waste by isotope dilution mass spectrometry

Yamamoto, Masahiko; Taguchi, Shigeo; Horigome, Kazushi; Kuno, Takehiko

Proceeding IAEA Symposium on International Safeguards; Building Future Safeguards Capabilities (Internet), 8 Pages, 2018/11

In this study, the single-column extraction chromatographic separation has been developed for analysis of U and Pu in highly active liquid waste by isotope dilution mass spectrometry (IDMS). The commercially available TEVA$$^{textregistered}$$ resin is selected as an extraction chromatography resin. The U is chromatographically separated from fission products (FP) elements by nitric acid while Pu(IV) is adsorbed on the resin. After that, Pu is eluted by reducing to Pu(III). The method has been successfully achieved the separation with yielding the enough recovery and sufficient decontamination factors for subsequent IDMS analysis. The column dose rate after the FP removal is decreased to the background. The analytical results obtained by the developed method are in a good agreement with those of the conventional method. It provides simple and rapid separation and expected that the method can be applied to join IAEA/Japan on-site analytical laboratory.

Journal Articles

Physical property evaluation of valve seal material at analytical radioactive liquid waste storage tanks in reprocessing facility

Goto, Yuichi; Yamamoto, Masahiko; Kuno, Takehiko; Inada, Satoshi

Nippon Hozen Gakkai Dai-15-Kai Gakujutsu Koenkai Yoshishu, p.489 - 492, 2018/07

Radioactive liquid waste from the Tokai Reprocessing Facility Analytical Laboratory is temporarily stored in intermediate waste storage tank by using receiving valves. Then, the liquid waste is transferred to liquid treatment facility by using liquid feed valves. The deterioration of the gasket part of these valves (leakage of waste liquid) was confirmed in 2004. Since then, the material of gaskets was changed from polyethylene to Teflon. In 2016, the gaskets were replaced by periodical update. Therefore, physical properties of used gaskets were investigated, and the relevance between radioactive level and degradation degree was evaluated.

JAEA Reports

Development of separation technique of Pu, Am, Np using solid phase extraction resin for the determination of impurity metal elements in plutonium nitrate solution by inductivity coupled plasma optical emission spectrometry

Taguchi, Shigeo; Yamamoto, Masahiko; Furuse, Takahiro*; Masaki, Yuji*; Kuno, Takehiko

JAEA-Technology 2018-005, 14 Pages, 2018/06

JAEA-Technology-2018-005.pdf:0.94MB

The method to remove Pu, Am and Np from plutonium nitrate solution recovered from spent nuclear fuel prior to ICP-OES measurement has been developed for the determination of 18 impurity metal elements (Fe, Cr, Ni, Mn, Al, Cd, V, Cu, Si, Zn, Mo, Sn, Ca, Mg, Na, Ag, Pb, B). In this method, two TRU resin packed columns were used for separation. In the first column, Pu and Am were mainly removed by adsorption. The recovered solution from the fist column was added to the second column after reduction of Np, and Am(III) and Np(IV) were removed by adsorption. The Pu nitrate solution (22g/L) of 2mL were treated by proposed method. The alpha emission nuclide was decreased to $$<$$5.8 Bq/mL in a solution diluted to 100mL. As a result of ICP-OES measurement, the recoveries of impurity metals separated by proposed method were almost 100%. This separation scheme can apply to the metal impurity elemental analysis in Pu nitrate solution recovered from spent nuclear fuel.

Journal Articles

Quantitative determination of total cesium in highly active liquid waste by using liquid electrode plasma optical emission spectrometry

Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo; Takamura, Yuzuru*; Surugaya, Naoki; Kuno, Takehiko

Talanta, 183, p.283 - 289, 2018/06

 Times Cited Count:1 Percentile:62.19(Chemistry, Analytical)

We develop a novel analytical method employing liquid electrode plasma optical emission spectrometry for measurement of total cesium in highly active liquid wastes. Limit of detection and limit of quantification are 0.005 mg/L and 0.02 mg/L, respectively. The method is validated and applied to the real samples.

Journal Articles

Online coupling of two-phase flow solvent extraction microfluidics with inductively coupled plasma mass spectrometry

Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo; Kuno, Takehiko; Surugaya, Naoki

Current Analytical Chemistry, 14(2), p.111 - 119, 2018/00

A direct coupling of two-phase flow solvent extraction microfluidics with ICP-MS for element-selective analysis is successfully established. Two-phase flow in microchannels of two combined glass chips for continuous extraction and back-extraction is stabilized through balancing the pressure by using an external coiled tube that functions as a flow resistor. The difference of fluid flow rate between microchannels and ICP-MS is adjusted by a proposed interface system including T-junction mixer and a switching valve. An online measurement of rhenium is successfully demonstrated. The calibration curve for Re is carried out in the range of 1 $$mu$$g/L to 20 $$mu$$g/L. The limit of detection is 0.2 $$mu$$g/L with a needed sample volume of one milliliter. Total time including extraction, back-extraction, and measurement is less than one hour. The development of the online coupling is a first step towards future applications to the selective measurement of highly radioactive elements.

Journal Articles

Replacement of the glove port equipped with glove box in Nuclear Fuel Reprocessing Facility

Horigome, Kazushi; Taguchi, Shigeo; Nishida, Naoki; Goto, Yuichi; Inada, Satoshi; Kuno, Takehiko

Nippon Hozen Gakkai Dai-14-Kai Gakujutsu Koenkai Yoshishu, p.381 - 384, 2017/08

no abstracts in English

Journal Articles

Design and application of greenhouse on the maintenance of analytical machineries in Tokai Reprocessing Plant

Suzuki, Yoshimasa; Tanaka, Naoki; Goto, Yuichi; Inada, Satoshi; Kuno, Takehiko

Nippon Hozen Gakkai Dai-14-Kai Gakujutsu Koenkai Yoshishu, p.385 - 389, 2017/08

Greenhouse is used in order to prevent diffusion of radioactive materials on the maintenance of machineries and decomposition of the analytical equipment such as glove box in Tokai Reprocessing Plant (TRP). The specifications of the greenhouse change depending on a risk of the radiation exposure, operation and environment. Design and application of original greenhouses in the analytical laboratory of TRP is summarized.

JAEA Reports

Preparation of uranium and plutonium mixed spike optimized for MOX analysis by isotope dilution mass spectrometry

Horigome, Kazushi; Taguchi, Shigeo; Yamamoto, Masahiko; Kuno, Takehiko; Surugaya, Naoki

JAEA-Technology 2017-016, 20 Pages, 2017/07

JAEA-Technology-2017-016.pdf:1.68MB

Mixed spikes of uranium and plutonium have been prepared for the determination of uranium and plutonium in dissolved MOX solution by isotope dilution mass spectrometry. Enriched uranium metal NBL CRM116 and plutonium metal NBL CRM126 were accurately weighed and then dissolved in nitric acid, respectively. Their dissolved solutions were mixed in a mass ratio of 1 to 2. The preparation values of uranium and plutonium were 1.0530 $$pm$$ 0.0008 mg/g (k=2) of uranium with a $$^{235}$$U relative mass fraction of 93.114 wt% and 2.0046 $$pm$$ 0.0019 mg/g (k=2) of plutonium with a $$^{239}$$Pu relative mass fraction of 97.934 wt%, respectively. The concentrations of uranium and plutonium in spike were confirmed by reverse isotope dilution mass spectrometry using tracer of $$^{233}$$U and $$^{242}$$Pu. Finally, the prepared spike was validated by parallel analysis of simulated sample of dissolved MOX solution. This spike was applied to measure the uranium and plutonium amount content of dissolved MOX solutions using isotope dilution mass spectrometry.

JAEA Reports

Application of controlled-potential coulometry as a primary method for the characterization of plutonium nitrate solutions being used for reference materials (Joint research)

Yamamoto, Masahiko; Holland, M. K.*; Cordaro, J. V.*; Kuno, Takehiko; Surugaya, Naoki

JAEA-Technology 2017-014, 63 Pages, 2017/06

JAEA-Technology-2017-014.pdf:4.38MB

In this study, the controlled-potential coulometry has been applied as a primary method for characterizing the Pu master solutions being used as alternative source material for IDMS spikes. The coulometry system compliance with ISO12183 has been used for measurement. It has been calibrated using equipment traceable to the SI units. Plutonium standard samples have been measured to confirm the accuracy. The relative standard deviation is below 0.05%. The results agree with the reference value within $$pm$$0.05%. It is found that the Pu can be precisely analyzed by the coulometry system. Then, the Pu nitrate solution, which has been purified from mixed oxide powder containing relatively high $$^{239}$$Pu, has been measured. The relative standard deviation is below 0.05%. The relative expanded uncertainty is less than 0.074% at the 95% confidence interval (k=2). It is indicated that coulometric assay of Pu is fit for the purpose of characterizing reference materials.

JAEA Reports

Report on analytical activities in potentially hazardous materials mitigation measures at the Plutonium Conversion Development Facility; 2015.12 $$sim$$ 2016.10

Horigome, Kazushi; Taguchi, Shigeo; Ishibashi, Atsushi; Inada, Satoshi; Kuno, Takehiko; Surugaya, Naoki

JAEA-Technology 2017-008, 14 Pages, 2017/05

JAEA-Technology-2017-008.pdf:1.15MB

The plutonium solution had been converted into MOX powder to mitigate the potential hazards of storage plutonium solution such as hydrogen generation at the Plutonium Conversion Development Facility. The plutonium conversion operations had been started in April, 2014, and had been finished in July, 2016. With respect to the samples taken from the conversion process, about 2,200 items of plutonium/uranium solutions and MOX powders had been analyzed for the operation control in the related analytical laboratories at the Tokai Reprocessing Plant. This paper describes the reports on analytical activities and related maintenance works in the analytical laboratories conducted from December, 2015 to October, 2016.

Journal Articles

Application of controlled-potential coulometry for the characterization of plutonium nitrate solutions being used for reference materials

Yamamoto, Masahiko; Holland, M. K.*; Cordaro, J. V.*; Kuno, Takehiko; Surugaya, Naoki

Dai-37-Kai Kaku Busshitsu Kanri Gakkai Nippon Shibu Nenji Taikai Rombunshu (CD-ROM), 9 Pages, 2017/02

Precise and accurate determination of plutonium is necessary. The high reliability is required for standard materials used in the plutonium determination. In this study, JAEA and SRNL have collaborated on a mission to apply controlled-potential coulometry as a primary method for characterizing the plutonium master solution being used for reference materials of isotope dilution mass spectrometry. The measurement cell and electrodes were upgraded and optimized compliance with ISO12183. The instruments were calibrated traceable to the SI. The samples of plutonium standard solution were measured to confirm the accuracy of the method. The results have been in good agreement with the reference values. Therefore, the plutonium solution which were purified from MOX powder have been characterized. The total measurement uncertainty was less than 0.07%. The results indicated that coulometry assay of plutonium are fit for the purpose of characterizing reference material.

JAEA Reports

Determination of metal impurities in MOX powder by direct current arc atomic emission spectroscopy; Application of standard addition method for direct analysis of powder sample

Furuse, Takahiro*; Taguchi, Shigeo; Kuno, Takehiko; Surugaya, Naoki

JAEA-Technology 2016-028, 19 Pages, 2016/12

JAEA-Technology-2016-028.pdf:1.79MB

Metal impurities in MOX powder obtained from uranium and plutonium recovered from reprocessing process of spent nuclear fuel are needed to be determined for its characterization. Direct current arc atomic emission spectroscopy (DCA-AES) is one of the useful methods for direct analysis of powder sample without dissolving the analyte into aqueous solution. However, the selection of standard material, which can overcome concerns such as matrix matching, is quite important to create adequate calibration curves for DCA-AES. In this study, we apply standard addition method using the certified U$$_{3}$$O$$_{8}$$ containing known amounts of metal impurities to avoid the matrix problems. The proposed method provides good results for determination of Fe, Cr and Ni at a significant quantity level contained in MOX samples.

JAEA Reports

Report on analytical activities in potentially hazardous materials mitigation measures at the Plutonium Conversion Development Facility; 2014.4 $$sim$$ 2015.12

Horigome, Kazushi; Suzuki, Hisanori; Suzuki, Yoshimasa; Ishibashi, Atsushi; Taguchi, Shigeo; Inada, Satoshi; Kuno, Takehiko; Surugaya, Naoki

JAEA-Technology 2016-026, 21 Pages, 2016/12

JAEA-Technology-2016-026.pdf:1.14MB

In order to mitigate potential hazards of storage plutonium in solution such as hydrogen generation, conversion of plutonium solution into MOX powder has been carried out since 2014 in the Plutonium Conversion Development Facility. With respect to the samples taken from the conversion process, about 3500 items of plutonium/uranium solutions and MOX powders have been analyzed for the operation control in the related analytical laboratories at the Tokai Reprocessing Plant. This paper describes the reports on analytical activities and related maintenance works in the analytical laboratories conducted from April 2014 to December 2015.

Journal Articles

Replacement of the glove box panel in Nuclear Fuel Reprocessing Facility

Masui, Kenji; Yamamoto, Masahiko; Kuno, Takehiko; Surugaya, Naoki

Nippon Hozen Gakkai Dai-13-Kai Gakujutsu Koenkai Yoshishu, p.25 - 30, 2016/07

no abstracts in English

Journal Articles

Physical property of seal-gasket for glove box panel in reprocessing facilities

Goto, Yuichi; Yamamoto, Masahiko; Kuno, Takehiko; Surugaya, Naoki

Nippon Hozen Gakkai Dai-13-Kai Gakujutsu Koenkai Yoshishu, p.31 - 34, 2016/07

Chloroprene rubber gaskets are often used to seal the glove box body and its panels. Such gaskets are deformed with compressive pressure and its elastic restoring force keeps sealing property. Therefore, gaskets play an important role in glove box sealing. However, physical properties of those used in glove box have not reported so far. In this study, hardness, elongation, tensile strength and compression set are investigated and its sealing performances are evaluated. The gaskets samples are taken from the glove box, which is used for 37 years. It is found that hardness, elongation and tensile strength of gaskets are changed due to the aging but its values are within the specification of chloroprene rubber. Also, the compression-set is less than the value that sealing performance is decreased. The results show that even the gaskets are used for long time, it has the property to keep sealing performances of glove box.

Journal Articles

Application of controlled-potential coulometery as a primary method for the characterization of plutonium nitrate solutions being used for large-size dry spike reference materials; Collaboration between JAEA and SRNL

Holland, M. K.*; Cordaro, J. V.*; Morales-Arteaga, M. E.*; Yamamoto, Masahiko; Kuno, Takehiko; Surugaya, Naoki

Proceedings of INMM 57th Annual Meeting (Internet), 10 Pages, 2016/07

Since 2007, the laboratory at the Japan Atomic Energy Agency (JAEA) and Savannah River National Laboratory (SRNL) have collaborated on a new mission to apply controlled-potential coulometry as a primary method for characterizating plutonium master solutions. Measurement results are being used to prepare traceable and certifiable large-size dry (LSD) spike standards for safeguards measurements by isotope dilution mass spectrometry. The collaboration activities performed by JAEA and SRNL were authorized and funded under the JAEA & United States NNSA/DOE Permanent Coordinating Group. This report will chronicle the collaboration activities of JAEA and SRNL, and provide the detail on the periodic coulometer component calibration, the coulometric plutonium measures and measure practices, including the uncertainty propagation for the most recent plutonium master solution used for LSD Spike preparation.

Journal Articles

Radionuclide release to stagnant water in the Fukushima-1 Nuclear Power Plant

Nishihara, Kenji; Yamagishi, Isao; Yasuda, Kenichiro; Ishimori, Kenichiro; Tanaka, Kiwamu; Kuno, Takehiko; Inada, Satoshi; Goto, Yuichi

Journal of Nuclear Science and Technology, 52(3), p.301 - 307, 2015/03

 Times Cited Count:10 Percentile:12.68(Nuclear Science & Technology)

After the severe accident at the Fukushima-1 nuclear power plant, large amounts of contaminated stagnant water have accumulated in turbine buildings and their surroundings. This rapid communication reports calculation of the radionuclide inventory in the core, collection of measured inventory in the stagnant water, and estimation of radionuclide release ratios from the core to the stagnant water. This evaluation is based on data obtained before June 3, 2011. The release ratios of tritium, iodine, and cesium were several tens of percent, whereas those of strontium and barium were smaller by one or two orders of magnitude. The release ratios in the Fukushima accident were equivalent to those in the TMI-2 accident.

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