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論文

Decontamination and solidification treatment on spent liquid scintillation cocktail

渡部 創; 高畠 容子; 小木 浩通*; 大杉 武史; 谷口 拓海; 佐藤 淳也; 新井 剛*; 梶並 昭彦*

Journal of Nuclear Materials, 585, p.154610_1 - 154610_6, 2023/11

 被引用回数:0 パーセンタイル:0.01(Materials Science, Multidisciplinary)

Treatment of spent scintillation cocktail generated by analysis of radioactivity is one of important tasks for management of nuclear laboratories. This study proposed a procedure consists of adsorption of radioactivity and solidification of residual liquid wastes, and fundamental performance of each step was experimentally tested. Batch-wise adsorption showed excellent adsorption performance of Ni onto silica-based adsorbent, and chelate reaction was suggested as the adsorption mechanism by EXAFS analysis. Alkaline activate material successfully solidified the liquid waste, and TG/DTA and XRD analyses revealed that the organic compounds exist inside the matrix. Only 1% of the loaded organic compounds were leaked from the matrix by a leaching test, and most of the organic compounds should be stably kept inside the matrix.

論文

Ion beam induced luminescence analysis of europium complexes in styrene-divinylbenzene copolymer-coated spherical silica by proton and argon ion beams irradiation

中原 将海; 渡部 創; 竹内 正行; 湯山 貴裕*; 石坂 知久*; 石井 保行*; 山縣 諒平*; 山田 尚人*; 江夏 昌志*; 加田 渉*; et al.

Nuclear Instruments and Methods in Physics Research B, 542, p.144 - 150, 2023/09

 被引用回数:0 パーセンタイル:0.02(Instruments & Instrumentation)

マイナーアクチニド回収のための抽出クロマトグラフィ技術において、荷電粒子誘起発光分析により様々な抽出剤を用いて調製した吸着材中のユウロピウム錯体構造の評価を行った。測定は、量子科学技術研究開発機構のイオン照射施設においてシングルエンド加速器から得られる陽子ビーム及びサイクロトロン加速器から得られるアルゴンイオンビームを利用して行った。本研究において、抽出剤の種類によって荷電粒子誘起発光スペクトルが変化することが確認され、これらの変化と錯体構造のとの相関について評価を行った。

論文

Evaluation of the remaining spent extraction solvent in vermiculite after leaching tests via PIXE analysis

荒井 陽一; 渡部 創; 長谷川 健太; 岡村 信生; 渡部 雅之; 武田 啓佑*; 福元 博基*; 吾郷 友宏*; 羽倉 尚人*; 塚原 剛彦*

Nuclear Instruments and Methods in Physics Research B, 542, p.206 - 213, 2023/09

 被引用回数:0 パーセンタイル:0.02(Instruments & Instrumentation)

Spent PUREX solvent, which mainly consists of tributyl phosphate (TBP) and normal dodecane, is generated by solvent extraction of Plutonium and Uranium in the spent nuclear fuel reprocessing. One of the treatment options for storage of the spent solvent is adsorption of the liquid into vermiculite. The organic liquid is considered to be trapped between layers of the vermiculite. Our previous experiments on the adsorption of spent solvent into the vermiculite have shown that some parts of loaded solvent gradually leaked out from the vermiculite. In order to investigate the adsorption mechanism and capacity, elution behavior of the loaded solvent into organic diluents were evaluated. A part of the loaded solvent was easily leaked into the diluent, while some solvent remained inside the particle even after the leaching test. In this study, the adsorption capacity of the vermiculite was evaluated through amount of remaining solvent after washing with diluents. The amount of the remaining solvent was analyzed by Particle Induced X-ray Emission (PIXE) on P contained in TBP. Peak intensity of P-K$$alpha$$ line depended on the washing condition, and the behavior of the amount of change in adsorbed P atom qualitatively agreed with the results of the leaching test.

論文

Improvement in the elution performance of an N,N,N',N-tetraoctyl diglycolamide impregnated extraction chromatography adsorbent using neodymium via micro-particle-induced X-ray emission analysis

高畠 容子; 渡部 創; 新井 剛*; 佐藤 隆博*; 柴田 淳広

Applied Radiation and Isotopes, 196, p.110783_1 - 110783_5, 2023/06

 被引用回数:0 パーセンタイル:0.01(Chemistry, Inorganic & Nuclear)

An adsorbent used for the recovery of trivalent minor actinides (MA(III); Am and Cm) from high level liquid waste generated from reprocessing of spent nuclear fuel was subjected to micro-PIXE analysis to improve its elution performance. The experimental adsorbent comprised SiO$$_{2}$$ particles, a polymer coating, and an TODGA. The particles to be analyzed were subjected to Nd adsorption and an elution operation, but Nd in the adsorbent was found to be uniformly distributed. This might have been caused by individual differences in the amount of impregnated TODGA. The remaining Nd species were not localized to a specific part of the adsorbent after the adsorption operation. Some Nd elements were retained in the adsorbent after elution, probably because of the poor diffusion of the mobile phase inside the adsorbent. An adsorbent having a different microstructure from the first was then evaluated, and rapid elution was observed on new adsorbent along micro-PIXE analysis

論文

Treatment of U contaminated waste generated from nuclear fuel fabrication process, 1; Ce(IV) recovery by temperature swing extraction with monoamides

岩本 敏広; 齋藤 まどか*; 高畠 容子; 渡部 創; 渡部 雅之; 成瀬 惇喜*; 塚原 剛彦*

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 4 Pages, 2023/05

モノアミド抽出剤と温度応答性ポリマーを用いたゲル化抽出技術のウラン廃棄物処理への適用性の検討を行った。異なる構造を有する3種類のモノアミド抽出剤を用いた模擬溶液の分離試験により、溶液中のCe(IV)をゲル化抽出法により選択的に回収されることが示された。これらの試験結果をもとに、ゲル化抽出法に適したモノアミド抽出剤を選定した。

論文

Development of engineering scale extraction chromatography separation system, 2; Spray drying granulation of silica support for adsorbent

長谷川 健太; 後藤 一郎*; 宮崎 康典; 安倍 弘; 渡部 創; 渡部 雅之; 佐野 雄一; 竹内 正行

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 5 Pages, 2023/05

JAEA has been working on development of extraction chromatography technology for recovery of trivalent minor actinides (MA(III): Am, Cm) from high-level radioactive waste generated in reprocessing of spent fuel. The technology utilizes porous silica particles with about 50 micrometre diameter for support of adsorbents. The particles are coated by styrene-divinylbenzene copolymer, and an extractant for MA recovery is impregnated into the polymer. Pressure drop of the packed column depends on characteristics of the particle (diameter, uniformity and pore size). Large pressure drop of the column is not favorable for safety assessment of the technology although a certain level of the pressure drop is indispensable for excellent separation performance. In this study, spray drying granulation experiments and fundamental characterization of the product particle were carried out to find optimal specs of the particle and conditions of the granulation operation.

論文

Ion beam induced luminescence spectra of europium complexes in silica-based adsorbent

中原 将海; 渡部 創; 石井 保行*; 山縣 諒平*; 山田 尚人*; 江夏 昌志*; 湯山 貴裕*; 石坂 知久*; 加田 渉*; 羽倉 尚人*

QST-M-39; QST Takasaki Annual Report 2021, P. 62, 2023/02

マイナーアクチニド回収のための抽出クロマトグラフィ法において、効率的にマイナーアクチニドを分離するために吸着材中の錯体構造解析に係る研究を行っている。本研究では、マイナーアクチニドの模擬物質としてEuを使用し、シリカ担持型吸着材にEuを吸着させた試料を調製した。吸着材中のEu錯体の荷電粒子誘起発光スペクトルを測定し、Eu錯体構造解析に向けた基礎データを取得した。

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, 9 Pages, 2023/00

 被引用回数:0 パーセンタイル:0.01(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

Design of MA(III)/Ln(III) separation process of extraction chromatography technology

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

Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5851 - 5858, 2022/12

 被引用回数:3 パーセンタイル:31.61(Chemistry, Analytical)

In this work, we have examined Ln(III) and MA(III) separation conditions by the extraction chromatography using HONTA adsorbent to decide the Ln(III)/MA(III) separation process fow. From the research results, we found the simulated element of Am(III) for HONTA adsorbent and the conditions to use it. In addition, Ln(III) and Am(III) (simulated element) separation experiments were carried out using the HONTA adsorbent packed column, we have determined the column separation conditions for Am(III) such as order of fow solution and fow rate.

論文

Harmless treatment of radioactive liquid wastes for safe storage in systematic treatment of radioactive liquid waste for decommissioning project

中原 将海; 渡部 創; 粟飯原 はるか; 高畠 容子; 荒井 陽一; 小木 浩通*; 中村 雅弘; 柴田 淳広; 野村 和則

Proceedings of International Conference on Nuclear Fuel Cycle; Sustainable Energy Beyond the Pandemic (GLOBAL 2022) (Internet), 4 Pages, 2022/07

高レベル放射性物質研究施設において高速炉燃料再処理技術,高レベル放射性廃棄物処分技術,核燃料サイクル技術に関する基礎研究に伴い様々な液体廃棄物が発生している。これらの試験において様々な試薬は使用されており、試験の過程で有害な物質が発生している。これらの放射性液体廃棄物を安全な状態で保管するために分解,溶媒抽出,沈殿,固化処理等により無害化処理に関する研究開発を実施している。本研究では、放射性液体廃棄物の無害化処理に係る研究開発の現状を報告する。

論文

Hybrid process combining solvent extraction / low pressure loss extraction chromatography for a reasonable MA(III) recovery process

佐野 雄一; 坂本 淳志; 宮崎 康典; 渡部 創; 森田 圭介; 江森 達也; 伴 康俊; 新井 剛*; 中谷 清治*; 松浦 治明*; et al.

Proceedings of International Conference on Nuclear Fuel Cycle; Sustainable Energy Beyond the Pandemic (GLOBAL 2022) (Internet), 4 Pages, 2022/07

TBPを利用した溶媒抽出法によるMA(III)+Ln(III)共回収フローシート及び低圧損操作が可能な大粒径多孔質シリカ担体を使用したHONTA含浸吸着材を用いた擬似移動層型クロマトグラフィによるMA(III)/Ln(III)分離フローシートを組み合わせたハイブリッド型のMA(III)回収プロセスを開発した。

論文

Acid dissociation constant of bis(2-ethylhexyl) hydrogen phosphate impregnated in a polymer layer coated on silica microparticles

宮川 晃尚*; 竹内 正行; 新井 剛*; 渡部 創; 佐野 雄一; 中谷 清治*

Bulletin of the Chemical Society of Japan, 95(4), p.566 - 568, 2022/04

 被引用回数:3 パーセンタイル:42.81(Chemistry, Multidisciplinary)

高分子相に含浸させた抽出剤のpKaが、架橋度や他の抽出剤の共存によって変化し、高分子相の疎水性が変化することを実証した。本成果は、新規な固体抽出吸着剤の開発に役立つと考えられる。

論文

Structural characterization by X-ray analytical techniques of calcium aluminate cement modified with sodium polyphosphate containing cesium chloride

高畠 容子; 渡部 創; 入澤 啓太; 塩飽 秀啓; 渡部 雅之

Journal of Nuclear Materials, 556, p.153170_1 - 153170_7, 2021/12

 被引用回数:1 パーセンタイル:16.35(Materials Science, Multidisciplinary)

The long-time experimental activities on pyroprocessing have generated waste eutectic salts contaminated with nuclear materials. After reprocessing tests, waste salts should be appropriately treated, with a focus on Cl disposal considering its corrosive nature. It is important to construct Cl confinement for the waste salts. Chlorapatite (Ca$$_{10}$$(PO$$_{4}$$)$$_{6}$$Cl$$_{2}$$) has great potential for Cl confinement due to Ca and P. The chemical reactivity of Cl will be drastically reduced if chlorapatite can be synthesized in calcium aluminate cement modified with sodium polyphosphate (CAP) containing CsCl. This study confirms the chemical state of Cl and metal elements in the cement by XRD, XPS, and XANES in the CAP containing CsCl. The analyses results suggest the existence of the Ca-Cl-Cs and Al-Cl-Cs bonds in CAP containing CsCl. The formation of the chemical bonds of Cl with metal elements might be one of important factors for the chlorapatite formation from the CAP containing CsCl.

論文

Development of MA separation process with TEHDGA/SiO$$_{2}$$-P for an advanced reprocessing

堀内 勇輔; 渡部 創; 佐野 雄一; 竹内 正行; 木田 福香*; 新井 剛*

Journal of Radioanalytical and Nuclear Chemistry, 330(1), p.237 - 244, 2021/10

 被引用回数:6 パーセンタイル:65.59(Chemistry, Analytical)

抽出クロマトグラフィ法を採用した高レベル放射性廃液からのMA分離技術の構築のためにTEHDGA吸着材の適用性をバッチ式吸着およびカラム試験により評価した。バッチ式吸着試験の結果より、TEHDGA吸着材はTODGA吸着材と比較すると核分裂生成物の除染性能が優れていることが確認された。さらにカラム試験の結果より、TEHDGA吸着材から希土類元素の全量溶離が確認されたためTEHDGAは吸着材としても性能は十分に発揮され、プロセスへの適用が期待できる。

論文

Oxidative decomposition of ammonium ion with ozone in the presence of cobalt and chloride ions for the treatment of radioactive liquid waste

粟飯原 はるか; 渡部 創; 柴田 淳広; Mahardiani, L.*; 大友 亮一*; 神谷 裕一*

Progress in Nuclear Energy, 139, p.103872_1 - 103872_9, 2021/09

 被引用回数:2 パーセンタイル:31.78(Nuclear Science & Technology)

To prevent unexpected accidents at nuclear facilities caused by accumulated ammonium nitrate in an aqueous liquid waste containing ammonium salts and nitric acid, NH $$_{4}$$ $$^{+}$$ in the liquid waste must be decomposed under mild reaction conditions. In this study, we investigated the oxidative decomposition of NH $$_{4}$$ $$^{+}$$ with O$$_{3}$$ at 333 K in the presence of a homogeneous Co$$^{2+}$$ catalyst and Cl$$^{-}$$ in the wide pH range of the test solution. The reaction behavior was greatly affected by pH of the test solution. In a basic solution at pH 12, high conversion of NH $$_{4}$$ $$^{+}$$ was obtained even in the absence of Co$$^{2+}$$ and Cl$$^{-}$$ and the main product was NO $$_{3}$$$$^{-}$$. However, Co$$^{2+}$$ and Cl$$^{-}$$ in the solution greatly enhanced the decomposition rate of NH $$_{4}$$ $$^{+}$$ in acidic to mild basic solutions (pH 1-8), while only low conversion of NH $$_{4}$$ $$^{+}$$ was observed unless both Co$$_{2+}$$ and Cl$$^{-}$$ were present. For the reaction with Co$$^{2+}$$ and Cl$$^{-}$$ in the solutions, NH$$_{4}$$ $$^{+}$$ was transformed mainly into chloramines (NH $$_{x}$$Cl $$_{3-x}$$, x = 1-3) by the reaction with HClO, which was formed by the reaction of Cl$$^{-}$$ with O$$_{3}$$ catalyzed by the homogeneous Co$$^{2+}$$ catalyst, and led to the high decomposition rate of NH$$_{4}$$ $$^{+}$$. Cl$$^{-}$$ suppressed the formation of the precipitate CoO(OH) during the reaction and consequently the Co$$^{2+}$$ catalyst stably existed in the reaction solution, which was another reason for the high decomposition rate of NH$$_{4}$$ $$^{+}$$ in the presence of Cl$$^{-}$$. Owing to the swift decomposition of NH$$_{4}$$ $$^{+}$$ under mild reaction conditions and small formation of secondary waste, the oxidative decomposition of NH$$_{4}$$ $$^{+}$$ in the presence of the homogeneous Co$$^{2+}$$ catalyst and Cl$$^{-}$$ is suitable and applicable for the treatment of the aqueous liquid waste containing ammonium salts and nitric acid.

報告書

高レベル放射性物質研究施設における放射性廃液の安定化処理

小木 浩通*; 荒井 陽一; 粟飯原 はるか; 渡部 創; 柴田 淳広; 野村 和則

JAEA-Technology 2021-007, 27 Pages, 2021/06

JAEA-Technology-2021-007.pdf:2.43MB

放射性物質取扱施設である高レベル放射性物質研究施設(CPF: Chemical Processing Facility)では、過去の試験や分析で発生した多種の廃液をホットセル及びグローブボックス内で保管してきた。2015年7月より、保管されている放射性廃液について、管理方法の適正化を図るべく、実廃液の安定化処理を進めている。また、分析廃液等の多種多様な試薬が混在する廃液については安定化処理が非常に困難であるため、大学等と共同でSTRAD(Systematic Treatments of Radioactive liquid wastes for Decommissioning)プロジェクトを発足させ、処理技術の研究開発を進めている。これらの実績は、他の放射性物質取り扱い施設においても保管する廃液の処理をより効率的かつ安全に進められることが期待できる。本書は、CPFで安定化処理を実施した実廃液の処理方法及び処理状況に関して報告するものである。

論文

Observation of Eu adsorption band in the CMPO/SiO$$_{2}$$-P column by neutron resonance absorption imaging

宮崎 康典; 渡部 創; 中村 雅弘; 柴田 淳広; 野村 和則; 甲斐 哲也; Parker, J. D.*

JPS Conference Proceedings (Internet), 33, p.011073_1 - 011073_7, 2021/03

中性子共鳴吸収イメージングを、抽出クロマトグラフィに使用するマイナーアクチノイド回収用CMPO/SiO$$_{2}$$-Pカラムで形成したEu吸着バンドの観測に適用した。軽水や重水で調製した湿潤カラムと乾燥吸着材を充填した乾燥カラムを比較し、中性子透過を評価した。中性子透過スペクトルから、乾燥カラムは45%、軽水調製カラムは20%、重水調製カラムは40%の中性子透過を確認した。得られた結果から、CMPO/SiO$$_{2}$$-Pカラムに形成したEu吸着バンドを観測するには、重水の使用によって、より鮮明になることを明らかにした。今後、カラム操作による吸着バンドのカラム内移行挙動を明らかにする。

論文

Microscopic analyses on Zr adsorbed IDA chelating resin by PIXE and EXAFS

荒井 陽一; 渡部 創; 大野 真平; 野村 和則; 中村 文也*; 新井 剛*; 瀬古 典明*; 保科 宏行*; 羽倉 尚人*; 久保田 俊夫*

Nuclear Instruments and Methods in Physics Research B, 477, p.54 - 59, 2020/08

 被引用回数:5 パーセンタイル:45.45(Instruments & Instrumentation)

Used PUREX process solvent generated from reprocessing process of spent nuclear fuel contains a small amount of U and Pu complexed with tributyl phosphate (TBP) or dibutyl phosphate (DBP). The radioactive nuclides should be removed from the solvent for safety storage or disposal. The iminodiacetic acid (IDA) type chelating resin was proposed as promising procedures for efficient recovery of the trapped cations in the solvent. In order to reveal the distribution and amount of Zr in the particle and local structure of Zr complex formed in the adsorbent, PIXE and EXAFS analyses on the Zr adsorbed chelating resin were carried out. Micro-PIXE analysis proved that it is an effectual method for quantitative analysis of trace adsorbed elements. Moreover, some of the adsorption sites were possibly occupied by the molecules. On the other hand, Zr-K edge EXAFS analysis suggested that extraction mechanism of Zr from the aqueous solution and the solvent was different.

論文

Structural characterization of Eu-HONTA complexes by IBIL and EXAFS analyses

渡部 創; 佐野 雄一; 岡田 諒*; 松浦 治明*; 羽倉 尚人*; 加田 渉*

Nuclear Instruments and Methods in Physics Research B, 477, p.60 - 65, 2020/08

 被引用回数:3 パーセンタイル:36.4(Instruments & Instrumentation)

抽出クロマトグラフィを用いたMA回収技術開発のためのHONTA含侵吸着材中に形成されるEu錯体の局所構造を、EXAFSとIBILとを組み合わせた手法により調査した。本分析により、吸着材中と溶媒中とで形成される錯体構造の微小な変化をとらえることができることが明らかとなった。

論文

Quantitative analysis of Zr adsorbed on IDA chelating resin using Micro-PIXE

荒井 陽一; 渡部 創; 大野 真平; 野村 和則; 中村 文也*; 新井 剛*; 瀬古 典明*; 保科 宏行*; 久保田 俊夫*

QST-M-23; QST Takasaki Annual Report 2018, P. 59, 2020/03

Radioactive spent solvent waste contains U and Pu is generated from reprocessing process of spent nuclear fuel. The nuclear materials should be removed from the solvent for safety storage or disposal. We are focusing on the nuclear materials recovery from spent solvent using imino diacetic acid (IDA) type chelating resin as a promising method. In order to reveal adsorbed amount of Zr, which is simulated of Pu, Micro-Particle Induced X-ray Emission (PIXE) was carried out. Micro-PIXE analysis succeeded in quantitative analysis on trace amount of adsorbed Zr from simulated spent solvent.

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