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

https://doi.org/10.1016/j.sab.2019.03.014

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).

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 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.

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.

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

https://doi.org/10.2174/1573411013666170421121927

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 g/L to 20 g/L. The limit of detection is 0.2 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.

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 0.0008 mg/g (k=2) of uranium with a U relative mass fraction of 93.114 wt% and 2.0046 0.0019 mg/g (k=2) of plutonium with a 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 U and 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.

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.

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

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.

Progress report of Japanese simulation research projects using the high-performance computer system Helios in the International Fusion Energy Research Centre

Ishizawa, Akihiro*; Idomura, Yasuhiro; Imadera, Kenji*; Kasuya, Naohiro*; Kanno, Ryutaro*; Satake, Shinsuke*; Tatsuno, Tomoya*; Nakata, Motoki*; Nunami, Masanori*; Maeyama, Shinya*; et al.

Purazuma, Kaku Yugo Gakkai-Shi, 92(3), p.157 - 210, 2016/03

http://www.jspf.or.jp/Journal/PDF_JSPF/jspf2016_03/jspf2016_03-157.pdf

The high-performance computer system Helios which is located at The Computational Simulation Centre (CSC) in The International Fusion Energy Research Centre (IFERC) started its operation in January 2012 under the Broader Approach (BA) agreement between Japan and the EU. The Helios system has been used for magnetised fusion related simulation studies in the EU and Japan and has kept high average usage rate. As a result, the Helios system has contributed to many research products in a wide range of research areas from core plasma physics to reactor material and reactor engineering. This project review gives a short catalogue of domestic simulation research projects. First, we outline the IFERC-CSC project. After that, shown are objectives of the research projects, numerical schemes used in simulation codes, obtained results and necessary computations in future.

Study on the behavior of radiolytically produced hydrogen in a high-level liquid waste tank of a reprocessing plant; Comparison between actual and simulated solutions

Kinuhata, Hiroshi*; Yamamoto, Masahiko; Taguchi, Shigeo; Surugaya, Naoki; Sato, Soichi; Kodama, Takashi*; Tamauchi, Yoshikazu*; Shibata, Yuki*; Anzai, Kiyoshi*; Matsuoka, Shingo*

Nuclear Technology, 192(2), p.155 - 159, 2015/11

https://doi.org/10.13182/NT15-15

Experiments using a small-scale apparatus with 30 ml actual high-level liquid waste from the Tokai Reprocessing Plant were carried out to show that the hydrogen concentration in the gas phase reaches a steady-state value of much less than 4% (lower explosive limit) in the absence of sweeping-air. The H concentration reached a steady-state value as was expected and it was compared with a value predicted from an equation with parameters which had been obtained using the simulated solution. Satisfactory agreement showed that the Pd-ion catalytic H consumption reaction previously found in the simulated solution proceeded equally well in the actual solution.