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論文

Quantitative imaging method of metallic lithium surface density using muonic X-rays

武田 伸一郎*; 桂川 美穂*; 高橋 忠幸*; 渡辺 伸*; Chiu, I.-H.; 二宮 和彦*; 新井 利彦*; 大西 光延*; 反保 元伸*; 下村 浩一郎*; et al.

Analytical Chemistry, 98(24), p.17618 - 17626, 2026/06

 被引用回数:0

Quantitative and non-destructive detection of metallic lithium (Li) deposition on Li-ion battery anodes is crucial for understanding degradation mechanisms and ensuring operational safety. Muonic X-ray spectroscopy (muXRS) is highly sensitive to light elements such as Li and enables probing of bulk materials; however, its application to practical devices has been limited by the lack of spatially resolved detection. In this study, we present an imaging system that extends muXRS by integrating a large-area silicon double-sided strip detector with a 3D-printed tungsten parallel-hole collimator. Using Li plate samples, we demonstrate quantitative two-dimensional imaging of metallic Li surface density with a spatial resolution of 5 mm. An image-processing method was developed to suppress crosstalk from carbon muonic X-rays and to correct beam non-uniformity, enabling reliable quantification. The system achieves a 1-sigma detection sensitivity of approximately 2.5 ug/mm$$^{2}$$, sufficient to detect localized Li accumulation. This approach extends muXRS from bulk-averaged analysis to spatially resolved measurement and provides a non-destructive tool for battery diagnostics.

論文

Automated flow electrolysis coupled with solid-phase extraction and ICP-MS/MS for rapid determination of neptunium-237

柳澤 華代; 松枝 誠; 岡 壽崇; 北辻 章浩

Journal of Radioanalytical and Nuclear Chemistry, 335(3), p.2091 - 2100, 2026/03

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

Conventional methods for determining neptunium-237 are labor-intensive and time-consuming, involving manual valence adjustments followed by chemical separation. These procedures are typically performed in open systems, which increases the risks of contamination, sample loss, and radiation exposure to workers. We developed a fully automated, semi-closed system that integrates flow electrolysis with solid-phase extraction and inductively coupled plasma-tandem mass spectrometry (ICP-MS/MS) to address these limitations. The system achieved a detection limit of 3.6 mBq/L (approximately 0.14 ng/L) with a 1 mL sample injection and a total analysis time of 25 min, enabling high-throughput analysis. Recovery tests using steel waste samples showed good agreement with the spiked values.

論文

Facile preparation of antiviral grafted fabrics based on silver-immobilized phosphate groups and evaluation of COVID-19 infections

松村 大樹; 辻 卓也; 瀬古 典明*; 他5名*

Journal of Radioanalytical and Nuclear Chemistry, 335(2), p.1543 - 1552, 2026/02

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

The COVID-19 pandemic has underscored the need for protective materials with rapid and durable antiviral properties. We developed silver (Ag)-immobilized fabrics via radiation-induced graft polymerization and tested their activity against SARS-CoV-2. The fabrics reduced 40,000 viral particles to below detection within one hour, showed no Ag leaching after 24 h in water, and retained complete antiviral performance after one year of storage. These findings demonstrate the long-term stability and strong potential of Ag-immobilized fabrics for industrial use in protective equipment.

論文

Development of HCl-free solid-phase extraction combined with ICP-MS/MS for rapid assessment of difficult-to-measure radionuclides, 4; Rapid determination of $$^{107}$$Pd in concrete rubble

太田 祐貴; Do, V.-K.; Banjarnahor, I. M.; 岩橋 弘之; 古瀬 貴広; 田中 康介

Journal of Radioanalytical and Nuclear Chemistry, 335(1), p.939 - 948, 2026/02

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

This paper presents an analytical method for detecting $$^{107}$$Pd in concrete using inductively coupled plasma tandem mass spectrometry (ICP-MS/MS). Palladium was purified through an HCl-free chromatographic process utilizing Ni-resin, which was optimized for high and stable chemical recovery. Palladium was effectively retained on the Ni-resin when treated with dilute nitric acid and was subsequently eluted with hot concentrated nitric acid. This approach improved elution efficiency and increased the recovery rate to over 90%. The determination of $$^{107}$$Pd via ICP-MS/MS was performed using NH$$_{3}$$ as a reaction gas. By measuring the mass shift of 51, corresponding to Pd(NH$$_{3}$$)$$_{3}$$$$^{+}$$ product ions, we successfully eliminated interference from the isobar $$^{107}$$Ag. The total interference removal factor for $$^{107}$$Ag reached approximately 10,000, demonstrating that the method is highly selective and reliable for quantifying $$^{107}$$Pd. The method detection limit for 107Pd in concrete matrices was estimated to be 0.05 Bq g$$^{-1}$$, indicating its sensitivity to detect low levels of the radionuclide, in compliance with environmental safety regulations. This method is now routinely used to monitor $$^{107}$$Pd in concrete samples collected from the Fukushima Daiichi Nuclear Power Station.

論文

Isotope-specific quantitative mapping of $$^{90}$$Sr at subfemtogram levels via online isotope dilution and laser ablation inductively coupled plasma tandem mass spectrometry

柳澤 華代; 松枝 誠; 古川 真*; 高貝 慶隆*

Analytical Chemistry, 97(50), p.27980 - 27987, 2025/11

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

The quantitative mapping of radioisotopes in solids is crucial for understanding their microscale localization and migration. However, conventional radiometric and mass spectrometric techniques are only capable of bulk measurements without spatial resolution. Imaging plates provide spatial resolution, but they lack selectivity and cannot quantify radioisotopes that only emit beta radiation, such as $$^{90}$$Sr. Here, the first system for isotope-specific quantitative mapping of a pure beta emitter is demonstrated that integrates online isotope dilution (ID) with laser ablation inductively coupled plasma tandem mass spectrometry (LA-ICP-MS/MS). In a case study, ultra-trace levels of $$^{90}$$Sr were accurately quantified without requiring matrix-matched certified reference materials (CRMs) for calibration or chemical separation. Severe isobaric/polyatomic interference (e.g., $$^{90}$$Zr$$^{+}$$, $$^{74}$$Ge$$^{16}$$O$$^{+}$$, $$^{89}$$Y$$^{1}$$H$$^{+}$$, and $$^{58}$$Ni$$^{16}$$O$$_{2}$$$$^{+}$$) was efficiently suppressed by O$$_{2}$$ reaction in a dynamic reaction cell, which greatly improved the abundance sensitivity and allowed sub-femtogram amounts of $$^{90}$$Sr to be quantitatively imaged. The background equivalent concentration (BEC) was 0.14 ng g$$^{-1}$$ (7.0 $$times$$ 10$$^{2}$$ Bq g$$^{-1}$$) per data point, and the measurement time was within 1 s. Validation with CRMs and $$^{90}$$Sr samples confirmed accuracy of 88$$sim$$116% relative to reference values. The proposed system is a versatile platform that can be applied to the practical mapping of radioactive solids, which has broad implications for nuclear waste disposal, environmental remediation, and radiation protection.

論文

Actinide separation by column method using polyvinylpolypyrrolidone

和田 一真*; 風間 裕行*; 阿部 千景*; 大西 貴士; 山本 昌彦; 田口 茂郎; 久野 剛彦; 前田 宏治; 出光 一哉*; 鈴木 達也*

Journal of Radioanalytical and Nuclear Chemistry, 334(11), p.8961 - 8968, 2025/11

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

市販のポリビニルポリピロリドン(PVPP)を質量分析の前処理として用いてアクチニドの分離を検討した。アクチニドとしては、ウラン、トリウム及びプルトニウムを用いた。硝酸中での吸着試験を行い、An(IV)とAn(VI)の吸着データを得た。また、PVPPを用いたカラム分離法により、An(III)/An(IV)/An(VI)の相互分離に成功した。さらに、炭酸イオンの導入により、U(VI)の溶出効率が向上した。本法は、アクチニドの質量分析のための相互分離法として応用できる可能性がある。

論文

Distribution of cesium-bearing microparticles in the paddy field and their effect on transfer factor of radioactive cesium for brown rice

辰野 宇大*; 二瓶 直登*; 吉村 和也

Journal of Radioanalytical and Nuclear Chemistry, 334(8), p.5719 - 5727, 2025/08

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

This study investigated the changes of radioactive cesium-bearing microparticles (CsMPs) deposition in the paddy field during the first year of resumed cultivation following the Fukushima Daiichi Nuclear Power Plant accident. Furthermore, we evaluate the contribution of CsMPs on a transfer factor (TF) of radiocesium (RCs) into brown rice. As a result, the accumulation of RCs and CsMPs in our study field was not observed. RCs concentration of brown rice was less than the shipping limit by defined by Japanese government. These suggest that there is little secondary contamination, and cultivation can be done safely. Furthermore, a significant effect of CsMPs on the TF was not found Cleary.

論文

A New analytical technique utilizing the PdI$$_{2}$$ target for measurement of $$^{129}$$I in environmental samples by accelerator mass spectrometry

本多 真紀; 高久 雄一*; 坂口 綾*; 松崎 浩之*; 末木 啓介*

Journal of Radioanalytical and Nuclear Chemistry, 334(8), p.5809 - 5820, 2025/08

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

$$^{129}$$I/$$^{127}$$I同位体標準とヨウ素水溶液を定量的に混合することで、AMSに最適なPdI$$_{2}$$の自家製標準物質シリーズを調製することができた。$$^{104,105}$$Pd$$^{4+}$$からの支配的な干渉は、精密にイオンを選別するElectrostatic cylindrical analyzerなどを調整することにより抑制することに成功した。その結果、海水とDolomite試料から調整したPdI$$_{2}$$について、その$$^{129}$$I/$$^{127}$$I原子数比はAgIとして調製した試料と一致した。新たな手法における前処理の時間は従来よりも33%短縮された。本研究はAMSにおける$$^{129}$$I分析法において通例とは違う新しい道を示すことに成功した。

論文

Assessment of suspended sediment and $$^{137}$$Cs sources during the flood event in the Fukushima river using $$^{13}$$C and $$^{14}$$C

中西 貴宏; 鶴田 忠彦; 舟木 泰智

Journal of Radioanalytical and Nuclear Chemistry, 334(7), p.5101 - 5107, 2025/07

 被引用回数:2 パーセンタイル:73.73(Chemistry, Analytical)

本研究では、放射性炭素同位体比$$Delta$$$$^{14}$$Cを指標として、福島第一原子力発電所事故後に河川に流出した懸濁態$$^{137}$$Csの発生源を特定した。出水時と平水時に懸濁物質を採取し、$$^{137}$$Cs濃度、$$Delta$$$$^{14}$$C、安定炭素同位体比を測定した。その結果、出水ピーク時に森林表層土壌流出の寄与が増加することが示された。さらに、流域における$$^{137}$$Csの沈着分布は、出水時の懸濁態$$^{137}$$Cs濃度の時間的変化に反映された。この手法は、放射性セシウム、炭素それぞれの動態を理解するために有用である。

論文

Development of HCl-free solid-phase extraction combined with ICP-MS/MS for rapid assessment of difficult-to-measure radionuclides, 3; Measurement of $$^{79}$$Se concentration in concrete rubble

Banjarnahor, I. M.; Do, V.-K.; 古瀬 貴広; 太田 祐貴; 田中 康介

Journal of Radioanalytical and Nuclear Chemistry, 334(7), p.4997 - 5006, 2025/05

 被引用回数:2 パーセンタイル:73.73(Chemistry, Analytical)

$$^{79}$$Se has been conventionally measured via radiometry. However, measuring $$^{79}$$Se this way is difficult due to its low specific radioactivity. Moreover, the measurement is time-consuming and susceptible to the radioactive interferences from highly radioactive nuclides ($$^{90}$$Sr, $$^{137}$$Cs, etc.) coexisting in the samples. ICP-MS/MS is widely known as a powerful technique to quantify difficult-to-measure radionuclides, which can effectively eliminate the interferences using a collision/reaction cell. In this research, a novel HCl-free chemical separation method was developed for separating Se from concrete matrices, followed by the selective measurement of Se concentration via ICP-MS/MS. $$^{79}$$Se was purified by stepwise chemical separation using anion exchange resin and activated alumina. The separation condition was optimized and evaluated. The chemical recovery of $$>$$ 85% was achieved. $$^{79}$$Se concentration was determined via ICP-MS/MS at m/z = 79 using ammonia gas as the reaction gas, and possible interferences such as those from the $$^{79}$$Br isobar and argon gas were effectively mitigated. A method limit of detection of 0.1 Bq g$$^{-1}$$ was achieved for the concrete rubble samples, making it a reliable tool for determining $$^{79}$$Se concentrations in concrete rubble collected from the Fukushima Daiichi Nuclear Power Station.

論文

Solvent extraction of tin in nitric acids; Evaluation of multiple extractants

伊藤 健吾*; 高橋 真*; 加藤 千図*; 福谷 哲*; 松村 達郎; 藤井 俊行*

Journal of Radioanalytical and Nuclear Chemistry, 334, p.2467 - 2475, 2025/02

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

本研究では、スズ、特に高レベル廃液に含まれるSn-126について、6種類の抽出剤による硝酸溶液からの溶媒抽出挙動について評価した。試験を行った抽出剤のうちHAAは高い効率を示したが、現状では工業的な応用に十分なデータは得られていない。塩酸を硝酸に加えた軽では、TBPとTEDTAにおいて、スズの分配比が1以上となった。しかしながら、工業的な応用に向けた実用的な課題と言う観点では、特に0.0008Mと言った低いスズ濃度におけるHAAによる抽出は、スズの回収についてより効果的である可能性がある。

論文

Development of Cs separation methods from large amounts of soil samples to determine the $$^{135}$$Cs/$$^{137}$$Cs isotope ratio

島田 亜佐子; 塚原 剛彦*; 野村 雅夫*; 武田 聖司

Journal of Radioanalytical and Nuclear Chemistry, 333(12), p.6297 - 6310, 2024/12

 被引用回数:2 パーセンタイル:40.43(Chemistry, Analytical)

Since the $$^{135}$$Cs and $$^{137}$$Cs concentration level of environmental soil in prefectures adjacent to Fukushima is low at about 5.5$$times$$10$$^{-15}$$$$sim$$ 6$$times$$10$$^{-13}$$ g g$$^{-1}$$, a large amount of soil is required to obtain sufficient amount to measure them precisely. Two Cs separation methods which allow to treat large amounts of leached soil solution was developed: 1) a continuous butch extraction method using calix[4]arene-bis(t-octylbenzo-crown-6) and 2) a combination method of selective Cs adsorption using ammonium phosphotangstate and anion-cation exchange resins. These methods were applied to low Cs concentration samples, and good precision of 0.8$$sim$$2.1% in the measurement of $$^{135}$$Cs/$$^{137}$$Cs isotope ratio was obtained.

論文

Solvent extraction of selenium in nitric acid; Evaluation of multiple extractants and proposal of a novel separation process

伊藤 健吾*; 川上 貴大*; 加藤 千図*; 福谷 哲*; 松村 達郎; 藤井 俊行*

Journal of Radioanalytical and Nuclear Chemistry, 333(10), p.5183 - 5189, 2024/10

 被引用回数:1 パーセンタイル:20.46(Chemistry, Analytical)

高レベル廃液からのウラン、プルトニウム、マイナーアクチノイド及び希土類元素の分離プロセスで使用される複数の抽出剤を用いて、硝酸溶液からのSe(VI)の溶媒抽出挙動を調べた。すべての抽出剤が分配比$$<$$1であったことから、プロセス中においてSeは残留水溶液中に残存することが明らかとなった。一方、希硝酸($$<$$ 2M HNO$$_{3}$$)、有機相としてオクタノール、濃硝酸(8M HNO$$_{3}$$)中において、抽出剤o-フェニレンジアミンではSeの分配比は1以上であった。濃硝酸(8M HNO$$_{3}$$)で逆抽出したところ、Seの新しい単一分離プロセスと回収の可能性が示唆された。

論文

Application of deep metric learning model to microscope image analysis for the determination of UOC samples in nuclear forensics analysis

木村 祥紀; 松本 哲也*; 山口 知輝

Journal of Radioanalytical and Nuclear Chemistry, 333(7), p.3541 - 3551, 2024/07

 被引用回数:1 パーセンタイル:20.46(Chemistry, Analytical)

This study discusses the application of a deep metric learning model based on a convolutional neural network to scanning electron microscope image analysis to determine UOC samples. One of the unique features of this technique is that it can detect a sample that comes from an unknown material not listed in the reference for comparison, in addition to the classification of a sample based on surface characteristics captured in the microscopic images. It was confirmed that the present technique could detect hypothetical unknown samples with $$>$$ 0.8 of Area Under the ROC Curve, and it can effectively provide preliminary observations in nuclear forensics analysis.

論文

Development of a non-destructive carbon quantification method in iron by negative muon lifetime measurement

二宮 和彦*; 久保 謙哉*; 稲垣 誠*; 吉田 剛*; 竹下 聡史*; 反保 元伸*; 下村 浩一郎*; 河村 成肇*; Strasser, P.*; 三宅 康博*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 333(7), p.3445 - 3450, 2024/07

 被引用回数:1 パーセンタイル:20.46(Chemistry, Analytical)

A novel nondestructive light element analysis method for bulk materials using muon beams was demonstrated. This method is based on the lifetime measurement of muons in a material and performed by measuring muon-decay electrons and identifying elements using the atomic number based on muon lifetimes. Muon irradiation on pure iron and two steel samples with known carbon contents was conducted to prepare a calibration curve for the quantitative analysis. We also performed a muon lifetime measurement for a Japanese sword and successfully determined its carbon content as 0.51 wt% using the calibration curve, without sample destruction.

論文

Investigation of adsorption mechanism of Mo(VI) by baker's yeast and applicability to the uranium liquid waste treatment process

荒井 陽一; 長谷川 健太; 渡部 創; 渡部 雅之; 箕輪 一希*; 松浦 治明*; 羽倉 尚人*; 勝木 健太*; 新井 剛*; 小西 康裕*

Journal of Radioanalytical and Nuclear Chemistry, 333(7), p.3585 - 3593, 2024/07

 被引用回数:1 パーセンタイル:12.78(Chemistry, Analytical)

Radioactive aqueous and organic liquid wastes contaminated by U are generated by solvent extraction of nuclear fuel materials in experiments of reprocessing technologies. Although incineration and denitrification/conversion processes are promising for treating such liquid waste, the installation of large equipment is essential. To give appropriate treatment procedures for radioactive liquid waste generated in nuclear facilities, STRAD (Systematic Treatments of RAdioactive liquid wastes for Decommissioning) project was started by Japan Atomic Energy Agency (JAEA) with several organizations. We are focusing on baker's yeasts for their excellent metal ions adsorption characteristics, easy handling and low prices. In order to optimize adsorption performance and operation procedures as the liquid waste treatment technology, adsorption performance of U has to be precisely investigated. In this study, adsorption performance of U and anion from nitric acid solution was investigated by batch-wise adsorption experiments.

論文

Water extraction of technetium-99m from neutron irradiated porous molybdenum dioxide pellet

Hu, X.*; 藤田 善貴; 土谷 邦彦; 福谷 哲*; 堀 順一*; 鈴木 達也*

Journal of Radioanalytical and Nuclear Chemistry, 333(11), p.6057 - 6063, 2024/05

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

難溶性である多孔質MoO$$_{2}$$ターゲットを使用した新しい$$^{99}$$Mo/$$^{99m}$$Tcジェネレータの製造方法を開発している。本方法では、水への溶解度の違いを利用してMoO$$_{2}$$から$$^{99m}$$Tcを抽出する。まず、作製した多孔質MoO$$_{2}$$ペレットをKUR(京都大学研究用原子炉)を用いて中性子照射した。照射した多孔質MoO$$_{2}$$を水へ浸漬させ、$$^{99m}$$Tcの抽出率を調べた。この結果、MoO$$_{2}$$から比較的低い$$^{99}$$Mo/$$^{99m}$$Tc比で$$^{99m}$$Tcが抽出され、MoO$$_{2}$$の水への溶解度は極めて低かった。さらに、$$^{99}$$Moの溶解度はその他のモリブデンの安定同位体よりも高く、(n,$$gamma$$)反応により生成された$$^{99}$$Moの溶解におけるホットアトム効果を明らかにした。本方法は、MoO$$_{2}$$ターゲットの再利用も可能で、製造プロセスの持続可能性を有するものであり、(n,$$gamma$$)反応で生成された$$^{99}$$Moを利用した水抽出による$$^{99}$$Mo/$$^{99m}$$Tcジェネレータの実現が期待できる。

論文

Development of a process for the separation of MA(III) from Ln(III) fission products using HONTA impregnated adsorbent

久保田 真彦*; Kim, S.-Y.*; Wu, H.*; 渡部 創; 佐野 雄一; 竹内 正行; 新井 剛*

Journal of Radioanalytical and Nuclear Chemistry, 333(5), p.2413 - 2420, 2024/05

 被引用回数:4 パーセンタイル:40.43(Chemistry, Analytical)

To minimize the use of organic solvents and achieve a selective adsorption separation of minor actinides (MA(III)) and Ln(III), adsorbents consisting of SiO$$_{2}$$-P particles impregnated with hexaoctylnitrilotriacetamide (HONTA) were prepared. Batch experiments were performed to evaluate the adsorption properties of the HONTA/SiO$$_{2}$$-P adsorbent for MA(III) and simulated fission products in HNO$$_{3}$$solution. The uniform distribution of Eu(III) on the adsorbent was confirmed via particle induced X-ray emission analysis, and X-ray photoelectron spectroscopy revealed that EuNO$$_{3}$$ was the adsorbed species. This study provides a simplified process for the separation of MA(III) using a HONTA/SiO$$_{2}$$-P packed column.

論文

$$^{137}$$Cs contamination of Japanese mustard spinach by resuspended particles in areas with different contamination conditions

辰野 宇大*; 吉村 和也; 二瓶 直登*

Journal of Radioanalytical and Nuclear Chemistry, 333(3), p.1089 - 1096, 2024/03

 被引用回数:0 パーセンタイル:0.00(Chemistry, Analytical)

Resuspended matters occur the secondary radioactive contamination of the crops in Fukushima Prefecture. We investigated the Cs-137 contamination derived from the resuspended matters to Japanese mustard spinaches in the multiple sites. In the less contaminated site, because Cs-137 of the surface ground soil was low, contamination of crops by the soil particles might be small. In the highly contaminated area, Cs-137 deposition of the soil particles might increase. However, the soil particles had no significant effect on Cs-137 contamination to crops. This was because the grown crop might cover the soil and reduce the Cs-137 deposition on the soil.

論文

Effect of $$^{226}$$Ra purity as a target for $$^{225}$$Ac production using a fast reactor

佐々木 悠人; 前田 茂貴

Journal of Radioanalytical and Nuclear Chemistry, 333, p.5987 - 5996, 2024/02

 被引用回数:2 パーセンタイル:40.43(Chemistry, Analytical)

研究者たちは、標的アルファ線治療のための$$^{225}$$Acが不足しているため、$$^{225}$$Acの代替製造法を求めている。廃棄物由来の$$^{226}$$Raを用いる製造法が検討されているが、$$^{226}$$Raの入手が問題である。そのため、ウラン鉱石から$$^{226}$$Raを回収する方法を検討する一方で、$$^{232}$$Th由来の$$^{228}$$Raが鉱物に混入することを懸念している。そこで、高速炉を用いた$$^{226}$$Ra核変換による$$^{225}$$Ac製造法における$$^{228}$$Ra汚染の影響を評価した。その結果、製造された$$^{225}$$Acには毒性の強い$$^{228}$$Acが混入していた。しかし、$$^{225}$$Acと$$^{228}$$Acの半減期の違いを利用して、5-8日間冷却した後、アクチニウムを化学分離することにより、純粋な$$^{225}$$Acが得られることがわかった。

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