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論文

Adsorption mechanism of Eu onto newly synthesized fluorous-compound-impregnating adsorbent

荒井 陽一; 渡部 創; 渡部 雅之; 新井 剛*; 勝木 健太*; 吾郷 友宏*; 藤川 寿治*; 武田 啓佑*; 福元 博基*; 保科 宏行*; et al.

Nuclear Instruments and Methods in Physics Research B, 554, p.165448_1 - 165448_10, 2024/09

 被引用回数:0 パーセンタイル:0.00(Instruments & Instrumentation)

Radioactive aqueous and organic liquid wastes contaminated by U and radioactive materials have been generated through solvent extraction experiments on nuclear fuel materials. Although incineration and denitrification / conversion processes are promising for treatment of such liquid wastes, installation of large equipment is essential. Treatment of liquid wastes generated from the reprocessing experiments is one of important tasks of Systematic Treatments of RAdioactive liquid wastes for Decommissioning (STRAD) project, and the recovery technologies of nuclear materials from the spent solvent has been developed. However, recovery of trace amounts of nuclear fuel material from aqueous solutions with wide pH range is still a challenging task. In our previous study, the porous silica particles with a high specific surface area bearing the iminodiacetic acid (IDA) functional group were revealed to be applicable to recover cations. Although the IDA group introduced adsorbents showed an excellent adsorption reaction from the aqueous solution, further improvement related to the adsorption amount is indispensable for application to the radioactive liquid treatment. In this study, fluorous ligands with IDA group were newly synthesized, and its complexation behavior with cations was investigated in order to understand the adsorption mechanism.

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:41.04(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

Kinetic analysis of mass transfer of Eu(III) in extractant-impregnated polymer-layered silica particle in multiple-ion distribution system

宮川 晃尚*; 林 直輝*; 岩本 響*; 新井 剛*; 長友 重紀*; 宮崎 康典; 長谷川 健太; 佐野 雄一; 中谷 清治*

Analytical Sciences, 40(2), p.347 - 352, 2024/02

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

複数のランタノイドイオンを含む錯体溶液中における単一抽出剤含浸高分子被覆シリカ粒子中のEu(III)分配機構を蛍光顕微分光法を用いて調べた。律速段階はEu(III)と2つの抽出剤分子との反応であった。得られた機構と速度定数は、Eu(III)溶液中でEu(III)が粒子に分配される単元素系の機構と一致した。

論文

Eu(III) transfer in single $$N,N,N',N'$$-tetraoctyldiglycolamide-impregnated polymer-coated silica particle using fluorescence microspectroscopy; Transfer mechanism and effect of polymer crosslinking degree

宮川 晃尚*; 高橋 拓海*; 崩 愛昌*; 岩本 響*; 新井 剛*; 長友 重紀*; 渡部 創; 佐野 雄一; 中谷 清治*

Analytical Sciences, 39(11), p.1929 - 1936, 2023/11

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

本研究では、単一のジグリコールアミド誘導体抽出剤(TODGA)を含浸させたポリマー被覆シリカ粒子におけるEu(III)分布を明らかにした。Eu(III)とポリマー層中の2つのTODGA分子との反応が律速過程であることが、速度定数(k$$_{1}$$ and k$$_{-1}$$)とEu(III)とHNO$$_{3}$$の濃度との間に相関がないことから明らかとなった。

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:0.00(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

Competitive distribution of europium and samarium based on reaction rate-limiting process in nitrilotriacetamide extractant-impregnated polymer-coated silica particles

宮川 晃尚*; 林 直輝*; 岩本 響*; 新井 剛*; 長友 重紀*; 宮崎 康典; 長谷川 健太; 佐野 雄一; 中谷 清治*

Bulletin of the Chemical Society of Japan, 96(9), p.1019 - 1025, 2023/09

 被引用回数:2 パーセンタイル:38.77(Chemistry, Multidisciplinary)

本研究では、ニトリロトリアセトアミド(NTA)抽出液を含浸させたポリマーコートシリカ単粒子において、Eu(III)とSm(III)のこれらのイオンを含む溶液中での物質移動機構を明らかにした。質量移動の律速過程は、NO$$_{3}$$$$^{-}$$イオンが関与しないイオンとNTA分子の反応過程であり、これは単一イオン分配系で得られたものと一致した。

論文

Kinetic mass transfer behavior of Eu(III) in nitrilotriacetamide-impregnated polymer-coated silica particles

宮川 晃尚*; 林 直輝*; 崩 愛昌*; 高橋 拓海*; 岩本 響*; 新井 剛*; 長友 重紀*; 宮崎 康典; 長谷川 健太; 佐野 雄一; et al.

Bulletin of the Chemical Society of Japan, 96(7), p.671 - 676, 2023/07

 被引用回数:4 パーセンタイル:62.38(Chemistry, Multidisciplinary)

HONTAおよびTOD2EHNTAとして知られるニトリロトリアセトアミド(NTA)抽出剤を含む単一ポリマー被覆シリカ粒子におけるEu(III)の分配機構を検討した。本研究は、「単一の抽出剤を含浸したポリマー被覆シリカ粒子」の機能性を評価・向上させるための貴重なアプローチを提供するものである。

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:1 パーセンタイル:41.04(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

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:5 パーセンタイル:72.25(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

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:28.95(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

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:7 パーセンタイル:69.06(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

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:7 パーセンタイル:60.47(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

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.

論文

Improvement in flow-sheet of extraction chromatography for trivalent minor actinides recovery

渡部 創; 先崎 達也; 柴田 淳広; 野村 和則; 竹内 正行; 中谷 清治*; 松浦 治明*; 堀内 勇輔*; 新井 剛*

Journal of Radioanalytical and Nuclear Chemistry, 322(3), p.1273 - 1277, 2019/12

 被引用回数:5 パーセンタイル:44.57(Chemistry, Analytical)

Extraction chromatography flow-sheet employing octyl(phenyl)-$$N,N$$-diisobutylcarbonoylmethylphosphine oxide (CMPO) and $$bis$$(2-ethylhexyl) hydrogen phosphate (HDEHP) extractants for trivalent minor actinide recovery was modified to improve column separation performance. Excellent trivalent minor actinides recovery performance was obtained by column separation experiments on nitric acid solution containing the trivalent minor actinides and representative fission product elements, i.e. recovery yields $$>$$ 93% with sufficient decontamination factors against the fission products. Those are the best performance which we have ever obtained by experiments inside hot cell.

論文

STRAD project for systematic treatments of radioactive liquid wastes generated in nuclear facilities

渡部 創; 小木 浩通*; 荒井 陽一; 粟飯原 はるか; 高畠 容子; 柴田 淳広; 野村 和則; 神谷 裕一*; 浅沼 徳子*; 松浦 治明*; et al.

Progress in Nuclear Energy, 117, p.103090_1 - 103090_8, 2019/11

AA2019-0193.pdf:1.29MB

 被引用回数:13 パーセンタイル:79.07(Nuclear Science & Technology)

A new collaborative research project for systematic treatments of radioactive liquid wastes containing various reagents generating in nuclear facilities was started from 2018 initiated by Japan Atomic Energy Agency. The project was named as STRAD (Systematic Treatments of RAdioactive liquid wastes for Decommissioning) project. Tentative targets to be studied under the project are aqueous and organic liquid wastes which have been generated by experiments and analyses in a reprocessing experimental laboratory of JAEA. Currently fundamental studies for treatments of the liquid wastes with complicated compositions are underway. In the STRAD project, process flow for treatment of ammonium ion involved in aqueous waste was designed though the inactive experiments, and decomposition of ammonium ion using catalysis will be carried out soon. Adsorbents for recovery of U and Pu from spent solvent were also developed. Demonstration experiments on genuine spent solvent is under planning.

論文

Extraction mechanism of lanthanide ions into silica-based microparticles studied by single microparticle manipulation and microspectroscopy

大高 稔紀*; 佐藤 辰巳*; 大野 真平; 名越 航平; 安倍 諒治*; 新井 剛*; 渡部 創; 佐野 雄一; 竹内 正行; 中谷 清治*

Analytical Sciences, 35(10), p.1129 - 1133, 2019/10

 被引用回数:9 パーセンタイル:36.59(Chemistry, Analytical)

Single porous silica microparticles coated with styrene-divinylbenzene polymer (SDB) impregnated with octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) were injected into an aqueous 3 mol/L nitric acid solution containing trivalent lanthanide (Ln(III)), as a high-level liquid waste model, using the microcapillary manipulation-injection technique; and the extraction rate of Ln(III), as an Ln(III)-CMPO complex, into the single microparticles was measured by luminescence microspectroscopy. The extraction rate significantly depended on the Ln(III), CMPO, or NO$$_{3}$$$$^{-}$$ concentration, and was analyzed in terms of diffusion in the pores of the microparticles and complex formation of Ln(III). The results indicated that the rate-determining step in Ln(III) extraction was the diffusion in the pore solution of the microparticles.

論文

Ion beam induced luminescence of complexes formed in adsorbent for MA recovery process

渡部 創; 片井 雄也*; 松浦 治明*; 加田 渉*; 江夏 昌志*; 佐藤 隆博*; 新井 剛*

Nuclear Instruments and Methods in Physics Research B, 450, p.61 - 65, 2019/07

 被引用回数:4 パーセンタイル:37.95(Instruments & Instrumentation)

Ion-beam induced luminescence (IBIL) analysis on MA recovery adsorbent was performed to give chemical states of complexes formed in the adsorbent as fundamental information for process design, and EXAFS analysis was also carried out to support discussions. The IBIL spectra of the binary extractants system seemed to be superposition of individual ones, however it has also original peaks. As intensities of those peaks rapidly decreased with iteration time of measurements and the original peaks were not observed for the adsorbent without charging Eu(III), they were attributed to complexes of Eu(III) with organic compounds. Contributions of CMPO and HDEHP extractants for Eu(III) extraction must be not only individual ones but also cooperative.

論文

Influences of pore and particle sizes of CMPO/SiO$$_{2}$$-P adsorbent on extraction chromatography process

渡部 創; 佐野 雄一; 三田 修平*; 桜井 翔太*; 新井 剛*

日本イオン交換学会誌, 30(1), p.8 - 16, 2019/01

In order to optimize operability of the adsorbents in the extraction chromatography system and to enhance the performance of the adsorbent, CMPO/SiO$$_{2}$$-P adsorbents with various pore and particle sizes were prepared, and characteristics of the adsorbents were evaluated through distribution coefficient, adsorption isotherm, adsorption rate, and breakthrough/elution behavior. Adsorption capacity was dominated not by the structure of the adsorbent but by amount of the extractant impregnated. The adsorbent with the largest pore size were revealed to show quick elution with short tail. Enlargement in the pore size must be one of the most effective improvements of the adsorbents to enhance the adsorption/elution performance. Adsorbent with particle size of more than 200 $$mu$$m formed channeling or voids inside the bed. They are suspected to lead slow adsorption/elution behavior, and smaller adsorbents must be desirable in the respect of performance of the column.

論文

Analysis on adsorbent for spent solvent treatment by micro-PIXE and EXAFS

荒井 陽一; 渡部 創; 大野 真平; 中村 雅弘; 柴田 淳広; 中村 文也*; 新井 剛*; 瀬古 典明*; 保科 宏行*; 羽倉 尚人*; et al.

International Journal of PIXE, 29(1&2), p.17 - 31, 2019/00

PUREX再処理等の試験研究により、U, Puを含む廃溶媒が発生し、安全な保管や廃棄の観点から、廃溶媒からの核燃料物質の回収は重要なプロセスである。そこで、Pu(IV)の模擬としてZr(IV)を用いて模擬廃溶媒を調製し、固体吸着材による回収法を検討し、イミノ二酢酸を導入した吸着材が廃溶媒中からの核燃料物質回収に有効であるとの結果を得ている。実用化に向けては吸着量の向上が課題であったことから、イミノ二酢酸の導入量を増加させるためにポリマーを被覆した多孔質シリカの利用を検討し、そのポリマーにイミノ二酢酸を導入することで吸着材を合成した。合成した吸着材について、廃溶媒処理への適用性を評価するためには、吸着能力と吸着メカニズムを明らかにする必要がある。そこで、微量元素の測定が可能であるマイクロPIXE分析に着目し、吸着したZrの分布や量を測定することで、吸着材に導入したイミノ二酢酸基の利用効率を評価した。また、吸着材中のイミノ二酢酸に吸着したZr周りの局所構造を明らかとするためにEXAFS分析を実施した。それぞれの分析結果から、本件で合成した吸着材は溶媒中でもZrと吸着反応を示すことを確認したが、沈殿と推察される粒子が観察され、吸着材の合成方法の更なる改善が必要である。

181 件中 1件目~20件目を表示