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報告書

革新的水質浄化剤の開発による環境問題低減化技術の開拓(委託研究); 令和2年度英知を結集した原子力科学技術・人材育成推進事業

廃炉環境国際共同研究センター; 信州大学*

JAEA-Review 2021-051, 81 Pages, 2022/01

JAEA-Review-2021-051.pdf:4.03MB

日本原子力研究開発機構(JAEA)廃炉環境国際共同研究センター(CLADS)では、令和2年度英知を結集した原子力科学技術・人材育成推進事業(以下、「本事業」という)を実施している。本事業は、東京電力ホールディングス株式会社福島第一原子力発電所の廃炉等をはじめとした原子力分野の課題解決に貢献するため、国内外の英知を結集し、様々な分野の知見や経験を、従前の機関や分野の壁を越えて緊密に融合・連携させた基礎的・基盤的研究及び人材育成を推進することを目的としている。平成30年度の新規採択課題から実施主体を文部科学省からJAEAに移行することで、JAEAとアカデミアとの連携を強化し、廃炉に資する中長期的な研究開発・人材育成をより安定的かつ継続的に実施する体制を構築した。本研究は、研究課題のうち、令和2年度に採択された「革新的水質浄化剤の開発による環境問題低減化技術の開拓」の令和2年度の研究成果について取りまとめたものである。本研究は、日英国際共同研究により再利用可能なストロンチウムイオン用吸着剤を開発し、使用済み吸着剤の発生量の削減を目指すものである。本研究の基本的な戦略は、信州大学チーム(信州大)で作製した吸着剤を分子科学研究所チーム(分子研)と英国チームで構造解析し、その結果を信州大で得られた吸着性能と合わせて東北大学チーム(東北大)がデータ科学的に理論解析し、吸着性能の改善に向けた作製指針を導き出す。その結果を信州大にフィードバックすることで、新たな吸着剤の作製につなげていくというものである。また、吸着剤由来の廃棄物処理法についても英国チームで検討することで、吸着剤の製造から廃棄までの一貫した研究が可能である。令和2年度の成果についてであるが、信州大は予備研究で見出された材料作製法を様々な条件で検討し、得られた材料の粒径分布や機械的強度などの物性への影響を調べた。また、塩化ストロンチウム単一溶液や人工海水に塩化ストロンチウムを溶解させた模擬汚染水中のストロンチウムイオンの吸着実験を行い、ICP装置により濃度を測定して分配係数を計算し、イオン選択性を評価した。得られた材料を分子研と英国チームに送り構造解析を依頼すると共に、吸着機能結果を東北大に送りデータ解析を依頼した。

論文

Direct quantitation of $$^{135}$$Cs in spent Cs adsorbent used for the decontamination of radiocesium-containing water by laser ablation inductively coupled plasma mass spectrometry

浅井 志保*; 大畑 昌輝*; 半澤 有希子; 堀田 拓摩; 蓬田 匠; 北辻 章浩

Analytical Chemistry, 92(4), p.3276 - 3284, 2020/02

 被引用回数:2 パーセンタイル:41.67(Chemistry, Analytical)

福島第一原子力発電所の汚染水処理に使用されたCs吸着材を安全に処分するために、長寿命核種である$$^{135}$$Csの放射能を把握する必要がある。$$^{135}$$Csは、誘導結合プラズマ質量分析計(ICP-MS)で測定するが、通常、液体試料のみに対応しているため、廃Cs吸着材の場合、Csの溶離操作が不可欠となる。しかし、$$^{137}$$Csから放出される強い放射線が取り扱いを困難にする。そこで本研究では、固体試料の直接測定が可能なレーザーアブレーションICP-MSを用いて$$^{135}$$Cs/$$^{137}$$Csを測定し、$$^{137}$$Csの$$gamma$$線測定結果と合わせて、Cs吸着材中の$$^{135}$$Csを簡便かつ精確に定量する方法を開発した。方法の妥当性を確認するため、放射性セシウムを含む汚染水に市販のCs吸着材を浸漬させて模擬試料を調製し測定したところ、水試料の分析値と一致した。

論文

Characteristics of TPDN/SiO$$_{2}$$-P adsorbent for MA(III) recovery

小藤 博英; 渡部 創; 竹内 正行; 鈴木 英哉; 松村 達郎; 塩飽 秀啓; 矢板 毅

Progress in Nuclear Science and Technology (Internet), 5, p.61 - 65, 2018/11

Applicability of newly developed MA(III)/RE(III) separation extractant TPDN for the extractionchromatography technology was evaluated through series of fundamental characterizations. The adsorbentselectively extract $$^{241}$$Am from diluted high level liquid waste and sufficient performance for MA(III)/RE(III)separation process was confirmed. Durability and behavior in the vitrification process of the adsorbent alsosuggested that the new adsorbent can be employed as a material for reprocessing of spent fuels.

論文

Minor actinides recovery from irradiated fuel for SmART cycle test

竹内 正行; 佐野 雄一; 渡部 創; 中原 将海; 粟飯原 はるか; 小藤 博英; 小泉 務; 水野 朋保

Proceedings of 2017 International Congress on Advances in Nuclear Power Plants (ICAPP 2017) (CD-ROM), 6 Pages, 2017/04

SmART cycle test has been promoted for reduction of volume and radiotoxicity of vitrified waste. It is a fuel cycle test using small amount of minor actinides (MA) in irradiated FBR fuels. The plan includes U, Pu and MA partitioning, fuel fabrication, irradiation at FBR and post irradiation examination. In this paper, a series of radioactive tests for MA partitioning from the irradiated fuel were mainly focused. As treatment of the irradiated fuel, it was sheared and dissolved by hot nitric acid, and then, U, Pu and Np in the dissolved fuel solution are co-extracted by solvent extraction. Am and Cm in the raffinate are efficiently separated by chromatographic technique. The target of MA yield for this cycle test is more than 1g to fabricate MOX pellets bearing 5% MA. As the current status for the MA partitioning, we have successfully finished the shearing and dissolution of the irradiated FBR fuel and solvent extraction process and the two steps flowsheet for Am and Cm partitioning from the raffinate and denitration behavior of separation product solution was discussed.

論文

Encapsulation of cesium from contaminated water with highly selective facial organic-inorganic mesoporous hybrid adsorbent

Awual, M. R.; 宮崎 有史; 田口 富嗣; 塩飽 秀啓; 矢板 毅

Chemical Engineering Journal, 291, p.128 - 137, 2016/05

 被引用回数:166 パーセンタイル:99.43(Engineering, Environmental)

A novel macrocyclic ligand of di-o-benzo-p-xylyl-28-crown-8-ether (DOBPX28C8) was prepared and successfully anchored onto the mesoporous silica for the fabrication of mesoporous hybrid adsorbent (MHA) using direct immobilization approach and serving as an efficient adsorbent for Cs removal. The high amount of K (7.69 mM) was slightly affected the Cs adsorption because the hydration radius of K is close to the Cs than that of the other cation of Na. Also the Cs adsorption efficiency was more higher even in the presence of 1,025 fold K and 1,739 fold Na, respectively. The functional group of DOBPX28C8 ligand embedded onto the mesoporous silica exhibited more conformational freedom, and the benzene ring in para position was consolidated for pai-electron orientation with expanding the ring size of DOBPX28C8 for easy capturing with high selectivity and adsorption ability towards the Cs.

論文

A Reliable hybrid adsorbent for efficient radioactive cesium accumulation from contaminated wastewater

Awual, M. R.; 矢板 毅; 宮崎 有史; 松村 大樹; 塩飽 秀啓; 田口 富嗣

Scientific Reports (Internet), 6, p.19937_1 - 19937_10, 2016/01

AA2015-0789.pdf:1.31MB

 被引用回数:132 パーセンタイル:98.16(Multidisciplinary Sciences)

A novel macrocyclic ligand of $$o$$-benzo-$$p$$-xylyl-22-crown-6-ether (OBPX22C6) was developed and successfully immobilized onto mesoporous silica for the preparation of hybrid adsorbent. The benzene ring $$pi$$ electron is the part of crown ether of OBPX22C6 for easy orientation of the macrocyclic compound for making the $$pi$$ electron donation with Cs complexation. The results clarified that the Cs removal process was rapid and reached saturation within a short time. Considering the effect of competitive ions, sodium did not markedly affect the Cs adsorption whereas potassium was slightly affected due to the similar ionic radii. Due to its high selectivity and reusability, significant volume reduction is expected as this promising hybrid adsorbent is used for Cs removal in Fukushima wastewater.

論文

Schiff based ligand containing nano-composite adsorbent for optical copper(II) ions removal from aqueous solutions

Awual, M. R.; Eldesoky, G. E.*; 矢板 毅; Naushad, M.*; 塩飽 秀啓; Alothman, Z. A.*; 鈴木 伸一

Chemical Engineering Journal, 279, p.639 - 647, 2015/11

 被引用回数:185 パーセンタイル:99.32(Engineering, Environmental)

A novel Schiff base ligand based nano-composite adsorbent (NCA) was prepared for the detection and removal of copper (Cu(II)) ions in wastewater samples. Upon the addition of Cu(II) ions to NCA at optimum conditions, the clear color was visible to the naked-eye in the detection system. This NCA exhibited an obvious color change from yellowish to dark green in the presence of Cu(II) ions in aqueous solution. The NCA could detect the Cu(II) ions over other foreign ions with high sensitivity and selectivity. For adsorption behaviour, influences several factors such as solution pH, contact time, concentration for Cu(II) ion adsorption was investigated by batch experiment in detail. The results showed that neutral solution pH was suitable to get optimum Cu(II) ions adsorption.

論文

A Sensitive ligand embedded nano-conjugate adsorbent for effective cobalt(II) ions capturing from contaminated water

Awual, M. R.; 矢板 毅; 塩飽 秀啓; 鈴木 伸一

Chemical Engineering Journal, 276, p.1 - 10, 2015/09

 被引用回数:126 パーセンタイル:98.44(Engineering, Environmental)

The organic ligand of N,N(octane-1,8-diylidene)di(2-hydroxyl-3,5-dimethylaniline) was synthesized and anchored onto inorganic mesoporous materials by direct immobilization method for Co(II) ions capturing from waste samples. The interaction of this material with various metal ions was evaluated, and it exhibited distinct color change from whitish to green in the presence of Co(II) ions, detectable even to the naked-eye. The effects of solution pH, contact time, competing ions and initial concentration on Co(II) sorption on NCA were investigated under optimum conditions. The data also clarified that the NCA adsorbent is an efficient and eco-friendly adsorbent for Co(II) treatment. Therefore, the proposed adsorbent can be considered as a potential candidate for Co(II) ions monitoring and removal from wastewater in large-scale operations.

論文

Comparative study of Sr adsorbents for radioactive contaminated water on severe accident

高畠 容子; 柴田 淳広; 野村 和則

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.2099 - 2104, 2015/09

The radioactive contaminated water has accumulated at Fukushima Dai-ichi Nuclear Power Station after the severe damage by the events accompanying the earthquake and tsunami. The concentration of Ca in the accumulated water is higher than that of Sr. Because of their chemical similarity, the secondary radioactive waste from Sr decontamination process will contains Ca more than Sr. Therefore, the volume of the secondary waste will increase more unnecessarily. Three kinds of Sr adsorbents; SW-KAZLS, the Hydrous titanic acid and SrTreat, were characterized and assessed from the viewpoint of Sr decontamination for radioactive contaminated water. The amount of Sr in SW-KAZLS showed the highest Sr selectivity. Since the Hydrous titanic acid was the hardest adsorbent of three, it is applied well to adsorption tower. The amount of Sr in SrTreat was favorable, and it could be applied to decontamination for the radioactive contaminated water of low Sr concentration.

論文

Large-pore diameter nano-adsorbent and its application for rapid lead(II) detection and removal from aqueous media

Shahat, A.*; Awual, M. R.; Khaleque, M. A.*; Alam, M. Z.*; Naushad, M.*; Chowdhury, A. M. S*

Chemical Engineering Journal, 273, p.286 - 295, 2015/08

 被引用回数:221 パーセンタイル:99.61(Engineering, Environmental)

The detection and removal of lead (Pb(II)) ions in water is essential for both human health and the natural environment. This study reported the feasibility of the large-pore diameter nano-adsorbent for capturing low level Pb(II) ions from aqueous solutions in a batch system, in order to comply with the toxicity limit for discharging wastewaters. The proposed Pb(II) detection system has good characteristics with high sensitivity and selectivity, robustness, easy operation, portability and use of a small sample volume. The competing ions effect was assessed with spiked samples and the nano-adsorbent exhibited high selectivity to Pb(II) ions with optimum color formation and the detection procedure can be easily applied to rapid on-site Pb(II) ions monitoring.

論文

Functional ligand anchored nanomaterial based facial adsorbent for cobalt(II) detection and removal from water samples

Shahat, A.*; Awual, M. R.; Naushad, M.*

Chemical Engineering Journal, 271, p.155 - 163, 2015/07

 被引用回数:187 パーセンタイル:99.39(Engineering, Environmental)

Ligand anchored functional nanomaterials are increasingly gaining interest as efficient materials for various types of toxic pollutants. In this study, the organic ligand was densely anchored onto the mesoporous silica by the building-block approach as facial adsorbent, characterized and then examined for the cobalt (Co(II)) ion detection and removal from aqueous solutions. This study also examined the possibility of using facial adsorbent to remove low concentrations of Co(II) ions from water solution. The sorption isotherms fit the Langmuir sorption model well and the maximum Co(II) ion sorption capacity was 157.73 mg/g. The effective eluent of 0.20M HCl was used to elute the Co(II) from the facial adsorbent, and the adsorbent was simultaneously regenerated into the initial form after rinsing with water.

論文

Ultimate selenium(IV) monitoring and removal from water using a new class of organic ligand based composite adsorbent

Awual, M. R.; 矢板 毅; 鈴木 伸一; 塩飽 秀啓

Journal of Hazardous Materials, 291, p.111 - 119, 2015/06

 被引用回数:152 パーセンタイル:98.7(Engineering, Environmental)

This work reports the selenium (Se(IV)) detection and removal from water by ligand functionalized organic-inorganic based novel composite adsorbent. The adsorbent exhibited distinct color change in the presence of various concentrations of Se(IV). This was characterized by UV-vis spectroscopy, and the color change was observed by naked-eye observation. The data fitted well to the Langmuir isotherm model, and the maximum Se(IV) sorption capacity was 111.12 mg/g. The presence of diverse competing ions did not affect the Se(IV) sorption capacity, and the adsorbent had almost no sorption capacity for these coexisting ions, which suggests the high selectivity to Se(IV) ions.

論文

A Novel facial composite adsorbent for enhanced copper(II) detection and removal from wastewater

Awual, M. R.

Chemical Engineering Journal, 266, p.368 - 375, 2015/04

 被引用回数:311 パーセンタイル:99.8(Engineering, Environmental)

The soft donor atoms containing organic ligand was prepared and then successfully immobilized onto the ordered nanomaterials to form facial adsorbent for copper(II) ions removal from water. The soft donor atoms of this ligand are actively working to make a stable complex formation with Cu(II) at a neutral pH region. It is also noted that the organic ligand was acted as receptors and able to transfer chemical information into analytical signals by charge transfer transudation during the detection operation.

論文

Investigation of ligand immobilized nano-composite adsorbent for efficient cerium(III) detection and recovery

Awual, M. R.; Hasan, M. M.*; Shahat, A.*; Naushad, M.*; 塩飽 秀啓; 矢板 毅

Chemical Engineering Journal, 265, p.210 - 218, 2015/04

 被引用回数:179 パーセンタイル:99.3(Engineering, Environmental)

In this study, the organic ligand of 4-dodecyl-6-((4-(hexyloxy)phenyl)diazenyl) benzene-1,3-diol (DPDB) and mesoporous silica have been used to prepare the nano-composite adsorbent. The nano-composite adsorbent was fabricated by indirect immobilization of DPDB onto the mesoporous silica. The experimental data clarified that the Ce(III) was detected and adsorbed by the adsorbent at pH 2.50. The limit of detection for Ce(III) ions by the adsorbent was 0.12 microgram/L and the sorption capacity was 150.37 mg/g at optimum conditions. The proposed adsorbent allowed the sensitive, selective, easy to use, cost-effective, high efficiency, fast kinetics and stable capturing of Ce(III) ions even in the presence of diverse competing ions.

論文

Organic-inorganic based nano-conjugate adsorbent for selective palladium(II) detection, separation and recovery

Awual, M. R.; Hasan, M. M.*; Znad, H.*

Chemical Engineering Journal, 259, p.611 - 619, 2015/01

 被引用回数:158 パーセンタイル:99.03(Engineering, Environmental)

The functional group containing organic ligand was developed and then successfully anchored onto mesoperous silica for the preparation of nano-conjugate adsorbent. After fabrication, the ligand kept open functionality for capturing Pd(II) under optimum conditions. The adsorbent exhibited the distinct color formation after adding the Pd(II) ions both in solid and liquid states. The base metal of Cu(II) and Zn(II) did not hamper the Pd(II) sorption ability of adsorbent in the acidic pH region. Therefore, it was expected that the Pd(II) could be separated from other hard metal ions by the adsorbent. Therefore the proposed adsorbent can be considered as a potential candidate for Pd(II) capturing from waste samples.

論文

Colorimetric detection and removal of copper(II) ions from wastewater samples using tailor-made composite adsorbent

Awual, M. R.; Hasan, M. M.*

Sensors and Actuators B; Chemical, 206, p.692 - 700, 2015/01

 被引用回数:178 パーセンタイル:99.77(Chemistry, Analytical)

The nitrogen donor ligand was functionalized with polarable mesoporous silica as composite adsorbent, by a cost-effective and environmentally friendly procedure, for highly selective Cu(II) ions detection and removal from water. The composite adsorbent permitted fast and specific Cu(II) ions capturing via colorimetric naked eye detection based on stable complexation mechanism. The adsorbent was selective toward Cu(II) as shown by a light yellow to green color change. This was characterized by UVvis spectroscopy and the color change was observed for the visual detection of Cu(II) ions. The data also confirmed that the adsorbent is a cost-effective and environmentally friendly procedure for Cu(II) treatment.

論文

Adsorption properties of styrenesulfonate-grafted fibrous metal adsorbent

植木 悠二; 佐伯 誠一; 瀬古 典明

日本イオン交換学会誌, 25(4), p.99 - 104, 2014/11

The dynamic adsorption/elution properties of an ethyl p-styrenesulfonate (EtSS)-based fibrous graft adsorbent having sulfonic acid (SO$$_{3}$$H) groups were evaluated by column-mode adsorption/elution tests for various cations. The EtSS-based fibrous graft adsorbent could work to capture various cations rapidly even under high flow rate conditions, compared with a commercial granular resin. The reason for this difference of adsorption rates was thought to be that the target ions were easily and rapidly transported near the SO$$_{3}$$H groups of graft chains by fluid convection. The affinity order of the fibrous graft adsorbent for cations depended on the cationic size and valence. It was found that the EtSS-based fibrous graft adsorbent preferentially adsorbed more multiply-charged cations having a larger cationic radius. The adsorbed cations could be easily eluted and concentrated by 1 M HNO$$_{3}$$ aqueous solution, and the recovery of each cation was reached over 90%. Based on the above results, it was found that the EtSS-based fibrous graft adsorbent could be available as a sophisticated metal adsorbent in the industrial processes.

論文

Functionalized novel mesoporous adsorbent for selective lead(II) ions monitoring and removal from wastewater

Awual, M. R.; Hasan, M. M.*; Shahat, A.*

Sensors and Actuators B; Chemical, 203, p.854 - 863, 2014/11

 被引用回数:133 パーセンタイル:99.17(Chemistry, Analytical)

In this study, we designed ligand immobilized mesoporous adsorbent for ultra-trace Pb(II) monitoring and removal from wastewater. This adsorbent exhibited the large surface area-to-volume ratios and uniformly shaped pores in case cavities, and its active sites kept open functionality to taking up Pb(II). The data revealed that the adsorbent was able to detect the ultra-trace Pb(II) ions with high sensitivity and selectivity by charge transfer transduction mechanism. Then the adsorbent proved to have an efficient ability for continuous Pb(II) monitoring and removal even on-site and in situ chemical analyses.

論文

A Novel ligand based dual conjugate adsorbent for cobalt(II) and copper(II) ions capturing from water

Awual, M. R.; 矢板 毅; 岡本 芳浩

Sensors and Actuators B; Chemical, 203, p.71 - 80, 2014/11

 被引用回数:136 パーセンタイル:99.2(Chemistry, Analytical)

Organic and inorganic based conjugate materials are important in nanotechnology based on the high functionality and stable complex formation with target metal ions at optimum conditions. A new ligand immobilization based dual and tunable conjugate adsorbent was investigated under specific solution acidity for detection and removal of Co(II) and Cu(II) ions. Under the optimum conditions, the calibration graphs were the linear and detection limit which were 0.52 and 0.41 ppb for Co(II) and Cu(II), respectively. The removal efficiency was carried out as a function of solution pH, initial metal ions concentration, and co-existing diverse ions. Sorption equilibrium was well fitted to Langmuir isotherms and determined sorption capacity was 205.33 and 199.20 mg/g for Co(II) and Cu(II), respectively.

論文

Mesoporous silica based novel conjugate adsorbent for efficient selenium(IV) detection and removal from water

Awual, M. R.; Hasan, M. M.*; 井原 敏博*; 矢板 毅

Microporous and Mesoporous Materials, 197, p.331 - 338, 2014/10

 被引用回数:133 パーセンタイル:99.19(Chemistry, Applied)

Selenium is a very toxic element that at low concentration can affect human beings and living organisms. In this study, the ligand immobilized conjugate adsorbent was developed and selenium (Se(IV)) detection and removal from water were investigated. The conjugate adsorbent was successfully prepared by direct immobilization of organic ligand onto mesoporous inorganic silica. This technique achieved residual Se(IV) concentration less than 10 ppb, which is acceptable by water quality regulations. Therefore, the solid design adsorbent is efficient and cost-effective for selective Se(IV) detection and removal from water.

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