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論文

Effect of B$$_{4}$$C absorber material on melt progression and chemical forms of iodine or cesium under severe accident conditions

日高 昭秀

Insights Concerning the Fukushima Daiichi Nuclear Accident, 4; Endeavors by Scientists, p.341 - 356, 2021/10

Boron carbide (B$$_{4}$$C) used for BWR or EPR absorbers could cause phenomena that never occur in PWR with Ag-In-Cd absorbers during a severe accident (SA). B$$_{4}$$C would undergo a eutectic interaction with stainless steel and enhance core melt relocation. Boron oxidation could increase H$$_{2}$$ generation, and the change of liberated carbon to CH$$_{4}$$ could enhance the generation of CH$$_{3}$$I. HBO$$_{2}$$ generated during B$$_{4}$$C oxidation could be changed to CsBO$$_{2}$$ by combining it with cesium. This may increase Cs deposition into the RCS. There could be differences in the configuration, surface area, and stainless-steel to B$$_{4}$$C weight ratio between the B$$_{4}$$C powder and pellet absorbers. The present task is to clarify the effect of these differences on melt progression, and the iodine or Cs source term. Advancement of this research field could contribute to further sophistication of prediction tools for melt progression and source terms of the Fukushima Accident, and the treatment of CH$$_{3}$$I formation in safety evaluation.

論文

Re-evaluation of radiation-energy transfer to an extraction solvent in a minor-actinide-separation process based on consideration of radiation permeability

樋川 智洋; 津幡 靖宏; 甲斐 健師; 古田 琢哉; 熊谷 友多; 松村 達郎

Solvent Extraction and Ion Exchange, 39(1), p.74 - 89, 2021/00

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

マイナーアクチノイド分離プロセスの放射線に対する成立性を評価するうえで、抽出溶媒の吸収線量の予測は不可欠である。本論文では、溶媒抽出時に現れるエマルションなどの構造を考慮した吸収線量評価手法を提案する。モンテカルロ法に基づいた放射線輸送コードであるPHITSを活用し、高レベル放射性廃液からのマイナーアクチノイド一括回収するプロセスを対象として、抽出溶媒への放射線エネルギー付与シミュレーションを行った。シミュレーションの結果、アルファ線によるエネルギー付与量はエマルション構造に、ベータ線及びガンマ線については抽出に用いる装置サイズに依存することを示した。さらにこれまでの線量評価では評価されてこなかった透過力の高いガンマ線によるエネルギー付与がマイナーアクチノイドの大量処理を考えるうえで重要になることを示唆した。

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

Current status of the high intensity pulsed spallation neutron source at J-PARC

高田 弘

Plasma and Fusion Research (Internet), 13(Sp.1), p.2505013_1 - 2505013_8, 2018/03

大強度陽子加速器施設(J-PARC)のパルス核破砕中性子源は、以下に示す独自の特長を有するモデレータを用いて高強度かつ幅の狭いパルス状の冷中性子を供給している。独自の特長とは、(1)100%比率のパラ水素を用いることでピークが高くテイル成分の低い中性子パルスをつくる、(2)直径14cm、高さ12cmの円筒形状とすることで、50.8$$^{circ}$$という広い取り出し角度範囲で高強度の中性子を利用できる、(3)銀-インジウム-カドミウム合金製の中性子吸収材を使用し、幅が狭く、テイル成分の低い中性子パルスをつくる、というものである。実際、低出力運転時の測定によって、1MWの運転時には、結合型モデレータで4.5$$times$$10$$^{12}$$n/cm$$^{2}$$/s/srの中性子束が得られ、ポイズン型モデレータを使用する中性子実験装置(BL08)では$$Delta$$d/d 0.035%の優れた分解能が得られることを確認した。ここで、dは結晶試料内のある方向の格子面と中性子の入射方向とのなす角度に垂直な方向の面間隔を意味する。1MWで年間5000時間の運転を行うという目標の達成に向けて、現在、微少気泡を水銀ターゲットに注入し、ターゲット容器に生じるキャビテーション損傷を抑制する技術開発やターゲット容器構造を溶接部やボルト接続をできるだけ減らす設計改良を行っている。

論文

Characteristics of radiocesium contamination of dry riverbeds due to the Fukushima Daiichi Nuclear Power Plant accident assessed by airborne radiation monitoring

浅見 和弘*; 太田垣 貴啓*; 石田 睦司; 眞田 幸尚

Landscape and Ecological Engineering, 14(1), p.3 - 15, 2018/01

 被引用回数:1 パーセンタイル:11.51(Biodiversity Conservation)

The Great East Japan Earthquake that occurred on March 11, 2011 generated a series of massive tsunami waves that caused severe damage to the Fukushima Daiichi Nuclear Power Plant, following which a large amount of radioactive materials was discharged from the power plant into the environment. Given the recently developed technologies for unmanned helicopters and their potential application in airborne radiation monitoring, we developed a radiation monitoring system for aerial use. We then used unmanned helicopters to measure the radiation level in areas with soil contaminated by radioactive cesium emitted from the nuclear power plant to evaluate the ambient dose-rate distribution around the site. We found that in dry riverbeds near the nuclear power plant, the dose rate was higher than that in landside areas. In addition, we carried out soil sampling in dry riverbeds. The results did not contradict the results measured by unmanned helicopter. As a result, a possible scenario is that river sediment and adjacent soil containing radioactive materials were carried from the upstream to the downstream due to an event such as a rise in water caused by a typhoon, etc., and remained in the riverbed after the water drained away. The vertical profile of radioactive materials in the soil and the measurement results for river sediment at river mouth areas corroborated the scenario.

論文

Implementation of a low-activation Au-In-Cd decoupler into the J-PARC 1 MW short pulsed spallation neutron source

勅使河原 誠; 池田 裕二郎; 大井 元貴; 原田 正英; 高田 弘; 柿白 賢紀*; 野口 学*; 島田 翼*; 清板 恭一*; 村島 大亮*; et al.

Nuclear Materials and Energy (Internet), 14, p.14 - 21, 2018/01

 被引用回数:0 パーセンタイル:0.01(Nuclear Science & Technology)

J-PARCの1MWパルス中性子源では、中性子パルスの成形に用いるデカップラとして、異なる共鳴吸収材から構成し、1eVと高い中性子吸収エネルギーを有するAg-In-Cd合金を開発した。このデカップラによりパルス成形された中性子は、粉末解析の実験装置において最高分解能を更新したが、中性子照射によって生成される長半減期の108mAgの放射能が高いため使用済み機器の取扱においては短所であった。そこで、放射能を大幅に減らす代替材としてAuを使用したAu-In-Cd材の開発を行ってきた。しかしながら、実機のモデレータ・反射体に実用化する上で、大型のAu-In-Cd板と構造材のA5083材とをHIP接合し十分な接合強度を得ることが課題であった。本研究では、Au-In-Cd材の表面状態、大型化した熱容量の変化による接合部界面温度に関わる検討を行い、実規模大のHIP接合において、最適接合条件を見つけることができた。この結果、反射体へのAu-In-Cd材の実用化に成功し、中性子性能を損なわず、大幅な放射能低減の見通しを得た。

論文

Release behavior of Cs and its chemical form during late phase of Fukushima Daiichi Nuclear Power Plant accident

日高 昭秀; 横山 裕也

Proceedings of Symposium on Water Chemistry and Corrosion in Nuclear Power Plants in Asia 2017 (AWC 2017) (USB Flash Drive), p.29 - 42, 2017/09

福島第一原子力発電所事故後期に東海村で測定された空気中のCsの性状が3月30日にガス状から粒子状に変わったことに関し、B$$_{4}$$C制御材を用いたPhebus FPT3実験やWSPEEDIコードによるソースターム逆算の結果を参照して、CsOHがB$$_{4}$$C起源のH$$_{3}$$BO$$_{3}$$と反応して生成するCsBO$$_{2}$$が再蒸発したことが原因であること、また、CsBO$$_{2}$$は環境中に放出後、逆反応を起こし、H$$_{3}$$BO$$_{3}$$が水に溶けたことがBの測定を難しくしているとの仮説を提案した。本仮説に基づく計算は、3月20日以降の炉心冷却注水量の最適化に伴う温度上昇時の環境中への放出量増大と合わせ、放出挙動を的確に再現できたが、推論の実証が重要である。今後は、様々な測定データを詳細に分析し、Bの存在を確認することが重要と考える。

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

LET dependency of human normal dermal cells survival in carbon ion irradiation

吉田 由香里*; 溝端 健亮*; 松村 彰彦*; 磯野 真由*; 八高 知子*; 中野 隆史*; 舟山 知夫; 小林 泰彦; 金井 達明*

JAEA-Review 2014-050, JAEA Takasaki Annual Report 2013, P. 81, 2015/03

日本の炭素線治療において臨床線量を決定するために用いられているclinical RBE (cRBE)はexperimental RBE (eRBE)にscaling factorをかけたものである。eRBEはhuman salivary gland(HSG)細胞を用いたコロニー形成法によりlinear-quadratic(LQ)モデルで得られた$$alpha$$値および$$beta$$値から求められた各LETにおけるRBEが採用されており、これが全ての患者(すなわちすべての細胞および組織)における炭素線治療計画に反映されている。しかしながら、RBEは線量,線量率,細胞や組織の種類、エンドポイント、酸素化の程度などにより異なる。そこで、群馬大学重粒子線照射施設(GHMC)のLET 13$$sim$$80keV/$$mu$$m、および原子力機構TIARAのLET 108$$sim$$158keV/$$mu$$mの炭素線を用い、その線量分布を評価すると共に、ヒト正常皮膚細胞への照射を行い、得られたRBE値について過去のHSG細胞の結果と比較・解析した。

論文

B$$_{4}$$C制御材がシビアアクシデント時の炉心溶融過程およびヨウ素やセシウムの化学形に与える影響

日高 昭秀

日本原子力学会和文論文誌, 14(1), p.51 - 61, 2015/03

原子炉の制御材としてBWR等で使用されているB$$_{4}$$Cは、PWRで用いられているAg-In-Cd制御棒材では見られない現象をシビアアクシデント時に引き起こし、炉心の溶融過程、H$$_{2}$$発生量、ソースターム等に影響する。炉心の溶融過程では、B$$_{4}$$Cはステンレス被覆管と共晶反応を起こし、融点以下でステンレスを液化させて炉心溶融を促進する。H$$_{2}$$発生量では、Bが酸化して発生量を増加させるとともに、遊離したCはCH$$_{4}$$に変化し、ヨウ素と結合することにより、ガス状のCH$$_{3}$$Iを生成させる。また、酸化過程で生じたHBO$$_{2}$$はCsBO$$_{2}$$を生成させ、原子炉冷却系内へのCs沈着量を増加させる。当面の課題は、粉末状のB$$_{4}$$C制御棒ブレードと、ペレット状のB$$_{4}$$C制御棒では、形状や表面積、B$$_{4}$$Cとステンレスとの重量比等に差があり、そのことが実際の溶融進展やB$$_{4}$$Cの酸化挙動、あるいは放射性物質の化学形や環境中への放出にどのように影響するのかを解明することである。今後、この分野の研究を進展させることにより、福島事故の炉心溶融進展やソースタームの高精度予測、安全評価における有機ヨウ素の扱い等に有用な知見を提供すると期待される。

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