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Journal Articles

Quantitation of long-lived radionuclide by ICP-MS

Asai, Shiho*; Horita, Takuma

Bunseki Kagaku, 73(10-11), p.569 - 578, 2024/10

The accurate estimation of the quantities and composition of long-lived radionuclides in radioactive waste is crucial for assessing the long-term safety of its disposal. Traditionally, theoretical predictions of the quantities of long-lived radionuclides obtained from burn-up calculation codes with evaluated nuclear data have been used especially for the safety assessment of high-level radioactive waste. However, such nuclear data used in theoretical predictions have not been sufficiently validated due to the scarcity of the reported measurement data. In this study, we aim to contribute to the improvement of the reliability of theoretical predictions by confirming them with the measured quantities of long-lived radionuclides per unit mass of uranium in spent nuclear fuel, which are output data obtained from the burnup calculation code. This involves measuring the long-lived radionuclides present in nuclear fuel pellets used in commercial nuclear reactors. Specifically, we focused on $$^{93}$$Zr, $$^{107}$$Pd, and $$^{135}$$Cs, which can be effectively measured using an inductively coupled plasma mass spectrometer (ICP-MS). Besides the purpose of validating the nuclear data, this article also highlights viable measurement techniques for these radionuclides, along with examples demonstrating their applicability to long-lived radionuclides, including the preparation procedures for their measurement.

Journal Articles

Flow peak detection using penalized asymmetric least squares in on-line isotope dilution-laser ablation-inductively coupled plasma-mass spectrometry

Yanagisawa, Kayo; Yokota, Hiromi*; Fujimoto, Katsushige*; Takagai, Yoshitaka*

Bunseki Kagaku, 73(9), p.515 - 522, 2024/09

On-line isotope dilution-laser ablation-inductively coupled plasma-mass spectrometry (on-line ID-LA-ICP-MS) is capable of quantification for each point ablated by laser, then the quantitative mapping of elements can be also conducted by reconstruction of the obtained each point data. The volume of data obtained as flow peaks in this system as a flow injection analysis, will be multiplied by each data such as number of m/z, scan time, time resolution and measurement position, and the total amount of data is enormous, resulting in a large human power and time consumption for data processing. In this paper, an original application software using Python to improve the efficiency of data processing in on-line ID-LA-ICP-MS was developed. To discriminate between the time-to-peak intensity and the background noise, an automatic peak detection using penalized asymmetric least squares was developed.

Journal Articles

Rapid analysis of radioisotopes using inductively coupled plasma-mass spectrometry and future developments

Matsueda, Makoto; Takagai, Yoshitaka*

Bunseki (Internet), 2024(6), p.195 - 200, 2024/06

The analytical demand for radioisotopes (RI) contained in radioactive waste from the decommissioning of nuclear power plants, research activities and nuclear accidents is increasing. However, traditional analytical methods of RI are mostly complicated and time-consuming, it is necessary to be rapid, simple and automatic methods. This paper describes the rapid analytical techniques of inductively coupled plasma-mass spectrometry in recent years, which current technology, challenges and perspective for the future.

Journal Articles

Factor analysis and X-ray absorption spectroscopy; Application to determination of individual chemical species and compounds

Ikeda, Atsushi

Bunseki Kagaku, 73(4.5), p.147 - 159, 2024/04

Factor analysis (FA), one of the multivariate analysis methods that are frequently employed in chemometrics, is a powerful tool to extract physical/chemical information of pure components from the analytical data of the mixture of the components. Although FA has been applied mainly to the quantitative analysis in the field of analytical chemistry, its application to the qualitative analysis has been limited. This article aims at introducing FA to the qualitative analysis for determining the speciation/structure of individual chemical species/compounds by X-ray absorption spectroscopy (XAS). The fundamental concept to extract physically/chemically meaningful information from XAS-FA is described, and some reported studies using XAS-FA for the qualitative determination of chemical species/compounds are summarized.

Journal Articles

Development of a quantification method for Zr isotopes in solid samples by LA-ICP-MS for rapid analysis of Zr-93 in high-level radioactive wastes

Morii, Shiori; Yomogida, Takumi; Asai, Shiho*; Ouchi, Kazuki; Oka, Toshitaka; Kitatsuji, Yoshihiro

Bunseki Kagaku, 72(10.11), p.441 - 448, 2023/10

Rapid analytical method for the determination of Zr-93 in radioactive wastes has been developed. Laser ablation (LA)-ICP-MS was applied to the analysis of Zr isotopes in simulated high-level radioactive waste (HLW). Sample preparation time was dramatically reduced by using a DGA resin as the adsorbent for Zr. Direct quantification of Zr isotopes in this resin sample was carried out by LA-ICP-MS. Laser settings were optimized to obtain a reliable isotope ratio of the sample by LA-ICP-MS. Quantification of Zr isotopes in the simulated HLW solution by isotope dilution mass spectrometry (IDMS) was examined. The amount of Zr-90 in the sample obtained by IDMS corresponded to a value calculated from the given concentration of Zr in the sample within uncertainty. Thus, this method can be applied for the quantification of Zr-93 in radioactive wastes.

Journal Articles

What is neutron-induced prompt gamma-ray analysis?

Osawa, Takahito

Hoshaka Bunseki, (34), p.34 - 50, 2023/04

This paper describes the nomenclature, principles, advantages and disadvantages of prompt gamma-ray analysis, the configuration of the PGA installed in JRR-3, what kind of analysis can be performed with the PGA, and how to use the PGA, respectively.

Journal Articles

Recent progress of $$^{135}$$Cs concentration and $$^{135}$$Cs/$$^{137}$$Cs isotopic ratio measurement

Shimada, Asako

Bunseki Kagaku, 71(12), p.625 - 633, 2022/12

Cesium-135 is one of the important nuclides to assess the safe disposal of High Level Waste (HLW). Therefore, the calculation code and library to evaluate the $$^{135}$$Cs concentration in HLW have been improved through comparisons with experimental results. On the other hand, even basic data of $$^{135}$$Cs, such as its half-life, have large uncertainty. Because the $$^{135}$$Cs/$$^{137}$$Cs isotopic ratio suggests its origin and introduction date, the ratios in environmental samples are measured to study global fallout from nuclear weapons testing and nuclear accidents. Such measurement methods was attracted attention, in particular, after the accident at the Fukushima Daiichi Nuclear Power Station. Measurement of the $$^{135}$$Cs/$$^{137}$$Cs isotopic ratio in environmental samples was challenging because the radiocesium has a very low concentration and it co-exists with huge amounts of Ba isotopes, which are isobaric interfering nuclides, are co-exist. Chemical separation methods were developed to eliminate interfering nuclides and improve the performance of the mass spectrometer to enable the measurement of the ratios. In this review, the features of the $$^{135}$$Cs/$$^{137}$$Cs isotopic ratio for each origin and recent developments in measurement techniques are summarized.

Journal Articles

Quantitation of trace lanthanide and actinide ions in radioactive samples by capillary electrophoresis-laser-induced fluorescence detection

Haraga, Tomoko; Saito, Shingo*

Bunseki Kagaku, 70(12), p.671 - 679, 2021/12

We developed highly sensitive capillary electrophoresis-laser-induced fluorescence detection methods for lanthanide (Ln) and actinide (An) ions with small sample volume and low emission of waste, by which the radiation risk can be minimized. Specifically, determination of Nd ion in spent nuclear fuel, effective separation between Am and Cm ion, and specific detection of UO$$_{2}$$$$^{2+}$$ in real radioactive samples were achieved by molecular design of fluorescence probes composed of an aminocarboxylate chelating moiety, a fluorophore and a spacer, and unique separation mode based on dynamic ternary complexation. We found that there are appropriate combination of probe and ternary complexation for detection and separation of each Ln and An ions. For example, acyclic and macrocyclic hexadentate is suitable for Ln$$^{3+}$$, Am$$^{3+}$$ and Cm$$^{3+}$$, and planer tetradentate with $$pi$$ electron system is specific for UO$$_{2}$$$$^{2+}$$, with ppt-sub ppt level detection.

Journal Articles

Progress of analytical chemistry through the experience of the Fukushima Daiichi Nuclear Power Plant Accident

Matsueda, Makoto; Takagai, Yoshitaka*

Bunseki, 2021(4), p.160 - 161, 2021/04

no abstracts in English

Journal Articles

Proper methods for treatment and handling of real samples; Inland water

Mochizuki, Akihito

Bunseki, 2021(1), p.2 - 7, 2021/01

no abstracts in English

Journal Articles

Appreciate new century award

Shimada, Asako

Nihon Bunseki Kagakukai Kanto Shibu Nyusu, (31), p.7 - 8, 2021/00

I am very glad to win a prize, new century award of Kanto branch of The Japan Society for Analytical Chemistry. I deeply appreciate recommender and co-workers. The title of award was "Development of analytical method of difficult to measure nuclides in radioactive wastes", and especially development of analytical method for Am-242m, Mo-93, and I-129 was recognized. By measuring beta-ray of Am-242, which is progeny nuclide of Am-242m and having high intensity and shorter half-life, measuring time was shortened to approximately 1/20 compare to traditional method. Analyzed Mo-93 example was extremely few. When Mo-93 was analyzed via X-ray, Zr-93 and Nb-93m were the interfering nuclides, therefore, separation method of Mo from Zr and Nb was developed and the method was applied to the rubble sample collected at the Fukushima Daiichi Nuclear Power Station (FDNPS). Official method to measure I-129 in environmental samples were optimized to measure I-129 in the contaminated water collected at FDNPS.

Journal Articles

Improvement of adsorption performances of Sr adsorption fiber and investigation for realizing simple $$^{90}$$Sr analysis

Horita, Takuma; Asai, Shiho*; Konda, Miki; Matsueda, Makoto; Hanzawa, Yukiko; Kitatsuji, Yoshihiro

Bunseki Kagaku, 69(10/11), p.619 - 626, 2020/10

 Times Cited Count:0 Percentile:0.00(Chemistry, Analytical)

We have developed a Sr adsorption fiber for rapid analysis of $$^{90}$$Sr. The prepared Sr adsorption fiber has a Sr-extraction layer that densely retains a Sr-selective extractant, an 18-crown-6 ether derivative, on the fiber surface. Hydrophobic group-containing polymer chains embedded onto the surface of the fiber allow to form a hydrophobic phase, incorporating Sr-selective extractants. This unique surface structure provides high adsorption capacity, leading to rapid and highly efficient adsorption of Sr$$^{2+}$$. The adsorption capacity of the Sr adsorption fiber was 3 times higher than commercially available 18-crown-6 ether derivative-impregnated resin (Sr Resin). The equilibrium adsorption capacity of the Sr adsorption fiber was comparable to the Sr Resin. The retained $$^{90}$$Sr was finally determined by a GM counter. The total analysis time including the Sr adsorption and measurement was about 1 hour.

Journal Articles

On-site measurement of nuclear material by using the fast neutron direct interrogation method

Komeda, Masao

Bunseki, 2019(10), p.459 - 461, 2019/10

no abstracts in English

Journal Articles

Recent trend of the radionuclide analyses in bioassay

Tomita, Jumpei

Bunseki, 2019(3), p.112 - 113, 2019/03

no abstracts in English

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

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

Journal Articles

Development of separation technique for platinum group metals from radioactive liquid waste utilizing laser-induced particulate formation

Saeki, Morihisa*; Asai, Shiho; Oba, Hironori*

Bunseki, 2018(4), p.138 - 143, 2018/04

Platinum group metal (PGM) has attracted much attention in light of increasing demands in the industrial sector. A wide variety of techniques specialized for PGM separation, such as, solvent extraction, solid phase extraction, and molten salt electrolysis have been developed so far. Among such techniques, a newly developed separation technique based on laser-induced particulate formation can be a promising alternative to conventional ones. It enables non-contact and highly-selective separation with a simple operation. In this review, the research history and the basic mechanism of laser-induced particulate formation were outlined. Several applications were also mentioned, focusing on our latest research progress which achieved a world first quantitation of radioactive palladium in a spent nuclear fuel sample.

Journal Articles

Recovery of rare metals using nucleic acid bases and extractants immobilized by grafted polymer chains

Saito, Kyoichi*; Asai, Shiho

Bunseki Kagaku, 66(11), p.771 - 782, 2017/11

 Times Cited Count:1 Percentile:3.18(Chemistry, Analytical)

Recovery and purification of rare metals, which are essential ingredients for highly functional materials, generally comes with operational difficulty. In this study, we have developed polymer adsorbents specially designed for highly-efficient adsorption of rare metal ions and exhibited their practical adsorption performances. Radiation-induced graft polymerization, one of the effective modification techniques for polymers, was employed for preparing the proposed adsorbents. Among such adsorbents, a 6-nylon fiber with nucleic-acid base, adenine, on the surface of the fiber demonstrated specific adsorption of ruthenium and palladium ions. In addition, a 6-nylon fiber with an extractant HDEHP (bis (2-ethylhexyl) phophoric acid) that has high affinity for lanthanides, achieved higher separation speed than a commercially available HDEHP-impregnated resin.

377 (Records 1-20 displayed on this page)