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論文

Development of a D$$_2$$O/H$$_2$$O vapor generator for contrast-variation neutron scattering

有馬 寛*; 高田 慎一; 笠井 聡*; 大内 啓一*; 森川 利明*; 宮田 登*; 宮崎 司*; 青木 裕之; 岩瀬 裕希*; 廣井 孝介; et al.

Journal of Applied Crystallography, 56(6), p.1802 - 1812, 2023/12

 被引用回数:0 パーセンタイル:0.02(Chemistry, Multidisciplinary)

The contrast-variation technique in neutron scattering experiments plays a pivotal role in distinguishing partial structures within multi-component complexes, facilitating the elucidation of distinct sample constituents. This differentiation is achieved using different isotopes, namely hydrogen and deuterium, which possess varying neutron scattering characteristics. This study presents a novel vapor generator designed for neutron scattering experiments, enabling continuous control of the D$$_2$$O/H$$_2$$O ratio of the vapor. This feature is especially useful for contrast-variation studies. The generator features two saturators and four mass flow controllers, allowing for the rapid and independent generation of D$$_2$$O/H$$_2$$O vapors. Additionally, the incorporation of the two-temperature method ensures accurate dew point control within a margin of $$pm$$0.2$$^{circ}$$Cdp. This setup proves useful for conducting time-resolved experiments and can accelerate research on functional polymers, such as polymer electrolyte membranes for fuel cells, where water potential assumes critical importance.

論文

Flow filtration/adsorption and simultaneous monitoring technologies of radiocesium $$^{137}$$Cs in river water

榎本 一之*; 保科 宏行*; 笠井 昇*; 栗田 圭輔; 植木 悠二*; 長尾 悠人*; 尹 永根*; 鈴井 伸郎*; 河地 有木*; 瀬古 典明*

Chemical Engineering Journal, 460, p.141696_1 - 141696_9, 2023/03

 被引用回数:1 パーセンタイル:38.53(Engineering, Environmental)

本研究では、モリブドリン酸アンモニウム(AMP)を放射線グラフト重合した繊維状のCs吸着フィルターとCe:Gd$$_3$$Al$$_2$$Ga$$_3$$O$$_{12}$$シンチレータを用いた$$gamma$$線検出器を組み合わせて、連続水流中の$$^{137}$$Csの放射能濃度をその場で測定する方法を開発した。

論文

Layered structure in the crystalline adsorption layer and the leaching process of poly(vinyl alcohol) revealed by neutron reflectivity

宮崎 司*; 宮田 登*; 有馬 寛*; 吉良 弘*; 大内 啓一*; 笠井 聡*; 津村 佳弘*; 青木 裕之

Langmuir, 37(32), p.9873 - 9882, 2021/08

 被引用回数:5 パーセンタイル:35.86(Chemistry, Multidisciplinary)

We investigated the structure of the crystalline adsorption layer of poly(vinyl alcohol) (PVA) in hot water by neutron reflectivity in two cases: when the adsorption layer is exposed on the substrate by leaching the upper bulk layer and when it is deeply embedded between a relatively thick PVA film and substrate. In both cases, the PVA adsorption layer consists of three layers on the Si substrate. The bottom layer, consisting of amorphous chains that are strongly constrained on the substrate, is not swollen even in hot water at 90$$^{circ}$$C. The middle layer, consisting of amorphous chains that are much more mobile compared with those in the bottom layer, has no freedom to assume a crystalline form. Only the molecular chains in the top layer are crystallizable in the adsorption layer, leading to a heterogeneous layered structure in the film thickness direction. This layered structure is attributed to the crystallizable chains of PVA during the formation of the adsorption layer driven by hydrogen bonding. However, the structure and dynamics in the adsorption layer may differ in both cases because the molecular chains in the vicinity of the surface seem to be affected by surface effects even in the adsorption layer.

論文

Fine-structure analysis of perhydropolysilazane-derived nano layers in deep-buried condition using polarized neutron reflectometry

阿久津 和宏*; 吉良 弘*; 宮田 登*; 花島 隆泰*; 宮崎 司*; 笠井 聡*; 山崎 大; 曽山 和彦; 青木 裕之

Polymers (Internet), 12(10), p.2180_1 - 2180_10, 2020/10

 被引用回数:2 パーセンタイル:6.56(Polymer Science)

A large background scattering originating from the sample matrix is a major obstacle for fine-structure analysis of a nanometric layer buried in a bulk material. As polarization analysis can decrease undesired scattering in a neutron reflectivity (NR) profile, we performed NR experiments with polarization analysis on a polypropylene (PP)/perhydropolysilazane-derived SiO$$_{2}$$ (PDS)/Si substrate sample, having a deep-buried layer of SiO$$_{2}$$ to elucidate the fine structure of the nano-PDS layer. This method offers unique possibilities for increasing the amplitude of the Kiessig fringes in the higher scattering vector (Qz) region of the NR profiles in the sample by decreasing the undesired background scattering. Fitting and Fourier transform analysis results of the NR data indicated that the synthesized PDS layer remained between the PP plate and Si substrate with a thickness of approximately 109 ${AA}$;. Furthermore, the scattering length density of the PDS layer, obtained from the background subtracted data appeared to be more accurate than that obtained from the raw data. Although the density of the PDS layer was lower than that of natural SiO$$_{2}$$, the PDS thin layer had adequate mechanical strength to maintain a uniform PDS layer in the depth-direction under the deep-buried condition.

論文

Gas-flow humidity control system for neutron reflectivity measurements

有馬 寛*; 宮田 登*; 吉田 鉄生*; 笠井 聡*; 大内 啓一*; Zhang, S.*; 宮崎 司*; 青木 裕之

Review of Scientific Instruments, 91(10), p.104103_1 - 104103_7, 2020/10

 被引用回数:9 パーセンタイル:54.35(Instruments & Instrumentation)

We developed a novel humidity control system for neutron reflectivity measurements based on the two-way gas-flow method that can generate up to 85% relative humidity (RH) within a temperature range of 5-85$$^{circ}$$C. The system consists of a gas-flow-type humidity generator and a thermostatic sample chamber, each of which can independently control the temperature. The key features include rapid humidity response and long stable operation time. The humidity reaches equilibrium within 2 to 5 min during the humidity change, and the system exhibited acceptable stability over a three-day, nonstop experimental measurement duration, with a precision of $$pm$$1% RH at 85$$^{circ}$$C and 85% RH. The sample chamber is capable of measuring substrate samples with dimensions of up to 2-in. in diameter and 5-mm in thickness. We demonstrate the reflectivity data measured at a pulsed neutron facility, MLF BL17, in the Japan Proton Accelerator Research Complex. The combined use of this system with neutrons permits in situ, time-resolved studies of the swelling process of polyvinyl alcohol and adhesive materials.

論文

Development of a water purifier for radioactive cesium removal from contaminated natural water by radiation-induced graft polymerization

瀬古 典明*; 保科 宏行*; 笠井 昇*; 柴田 卓弥; 佐伯 誠一*; 植木 悠二*

Radiation Physics and Chemistry, 143, p.33 - 37, 2018/02

 被引用回数:16 パーセンタイル:84.46(Chemistry, Physical)

Six years after the Fukushima-nuclear accident, the dissolved radioactive cesium (Cs) is now hardly detected inenvironmental natural waters. These natural waters are directly used as source of drinking and domestic waters in disaster-stricken areas in Fukushima. However, the possibility that some radioactive Cs adsorbed on soil or leaves will contaminate these natural waters during heavy rains or typhoon is always present. In order for the returning residents to live with peace of mind, it is important to demonstrate the safety of the domestic waters that they will use for their daily life. For this purpose, we have synthesized a material for selective removal of radioactive Cs by introducing ammonium 12-molybdophosphate (AMP) onto polyethylene nonwoven fabric through radiation-induced emulsion graft polymerization technique. Water purifiers filled with the grafted Csadsorbent were installed in selected houses in Fukushima. The capability of the grafted adsorbent to remove Cs from domestic waters was evaluated for a whole year. The results showed that the tap water filtered through the developed water purifier contained no radioactive Cs, signifying the very effective adsorption performance of thedeveloped grafted adsorbent. From several demonstrations, we have commercialized the water purifier named "KranCsair".

論文

Evaluation of a cesium adsorbent grafted with ammonium 12-molybdophosphate

柴田 卓弥; 瀬古 典明; 天田 春代; 笠井 昇; 佐伯 誠一; 保科 宏行; 植木 悠二

Radiation Physics and Chemistry, 119, p.247 - 252, 2016/02

 被引用回数:12 パーセンタイル:74.16(Chemistry, Physical)

A fibrous adsorbent for radioactive cesium (Cs) removal has been developed by radiation induced graft polymerization. To apply the developed adsorbent to drinking water, the stability of adsorbent having high affinity for Cs ligand, ammonium 12-molybdophosphate (AMP), was evaluated. As a result, since a crosslinking structure was introduced onto the grafted AMP, it could be successfully satisfied the regulation of Food Sanitation Act. Finally, the Cs adsorbent was commercialized as water purifier named by "KranCsairtextregistered".

論文

水域に飛散したセシウムを捕集する材料の開発

瀬古 典明; 柴田 卓弥; 笠井 昇; 植木 悠二; 佐伯 誠一; 保科 宏行

放射線と産業, (138), p.9 - 12, 2015/06

福島の原子力発電所災害以降、環境資源材料研究グループでは環境中の水域に飛散した放射性物質のうち、特にセシウムに対して効果のある捕集材料の開発を進めてきた。これまでの実績から水に対して接触効率が良好で、取り扱いの簡便な不織布繊維を基材に用い、これにセシウムに対して親和性のある吸着基を量子ビーム技術を活用した放射線グラフト重合技術により導入した。材料の評価では、福島被災地の各所で実施したフィールドテストで評価を重ね、最終的には井戸水, 沢水を対象にした飲用水向けのモニター試験を進め、その良好な結果から給水器の発売に繋げた経緯について紹介する。

論文

Evaluation of antibacterial effect by using a fibrous grafted material loaded Ag ligand

柴田 卓弥; 瀬古 典明; 笠井 昇; 保科 宏行; 植木 悠二

International Journal of Organic Chemistry, 5(2), p.100 - 107, 2015/06

To obtain the safety of drinking water, an antibacterial material was prepared by loading Ag onto fibrous iminodiacetate (IDA) adsorbent, which was synthesized by radiation induced graft polymerization of a glycidyl methacrylate and subsequent chemical modification of the produced epoxy group to an IDA group(IDA-Ag). A total amount of loaded Ag on the IDA-Ag fabric was 0.4 mmol-Ag/g-fabric. As a result of evaluating antibacterial effects by the column mode water flow test with a stream water, the effective Ag concentration was monitored 0.05 ppm at irrespective of flow rate which was functioned to the antibacterial performance. The antibacterial effects for general bacteria were indicated until BV (BV: steam water volume/IDA-Ag fabric volume) 6,000, and for colitis germ legions were completely disinfected until BV 6,000.

論文

Development of an adsorbent for Cs removal synthesized by radiation-induced graft polymerization

柴田 卓弥; 瀬古 典明; 天田 春代; 笠井 昇; 佐伯 誠一; 保科 宏行; 植木 悠二

日本イオン交換学会誌, 26(1), p.9 - 14, 2015/01

It is important task for recovering of Cs from the contaminated area caused by the accident at the Fukushima Daiichi Nuclear Power Station. We developed a highly efficient Cs adsorbent by radiation grafting of ammonium 12-molybdophosphate (AMP) and crosslinking of grafted chains with a suitable crosslinker at the same time. As a result of the optimizaion, the Cs adsorbent with 1 mol% of polyethylene glycol dimethacrylate satisfied the specification as a water purifier. The resultant grafted Cs adsorbent could work to maintain the highly performance of Cs removal in the standard pH range for drinking water (from pH 5.8 to 8.6) and even in the presence of coexisting ions such as K, Ca, Mg, and Na.

論文

大型核融合実験装置JT-60Uの解体

池田 佳隆; 岡野 文範; 逆井 章; 花田 磨砂也; 秋野 昇; 市毛 尚志; 神永 敦嗣; 清野 公広; 久保 博孝; 小林 和容; et al.

日本原子力学会和文論文誌, 13(4), p.167 - 178, 2014/12

JT-60Uを超伝導トカマクJT-60SAに改造するため、JT-60U本体を解体した。JT-60Uは18年間の重水素運転により放射化されており、このJT-60Uの解体は、放射化した核融合装置の解体として我が国初の解体であった。全ての解体品は、将来のクリアランスの適用を考慮し、線量当量率や材料、重量などのデータを記録した。切断技術や保管技術などは、効率的に解体を行うための鍵であった。解体に要した人工数や解体品の放射化レベルなど、他の核融合装置で解体を行う際に有用となる情報を報告する。

論文

The Volume reduction method of radioactively-contaminated plant waste through extraction and removal of radioactive cesium

佐伯 誠一; 柴田 卓弥; 保科 宏行; 植木 悠二; 笠井 昇; 瀬古 典明

日本イオン交換学会誌, 25(4), p.170 - 175, 2014/11

After Fukushima Daiichi Nuclear Power Plant accidents, a lot of contaminated wastes have been produced by decontamination works at contaminated areas around Fukushima prefecture, Japan. At some temporary storage sites, it was found that contaminated leaching water was accumulated under stacks of contaminated "plant" wastes. To handle the wastes and the solution properly, decontamination tests of the leaching water were examined with molybdophosphate type cesium adsorbents synthesized by radiation-induced grafting method. At batch adsorption tests, 75% of radioactive cesium was successfully removed with cesium adsorbents. At column adsorption tests, radioactivity concentration of the leaching water could be reduced under provisional limit value up to around 500 times volume as large as an adsorbent volume. For development of volume reduction method of contaminated plant wastes, radioactive cesium extraction tests from the wastes and removal tests from the extracts were executed using contaminated oil cakes of sunflower seeds as a model of contaminated plant wastes. As a result, 65% of radioactive cesium was successfully extracted from the oil cakes to liquid phase, and more than 65% of radioactive cesium could be collected from the extract by grafted cesium adsorbents. These results showed a possibility of an application of these processes to volume reduction method for contaminated plant wastes.

論文

Recovery of scandium from hot spring water with graft adsorbent containing phosphoric groups

保科 宏行; 笠井 昇; 天田 春代; 高橋 牧克*; 田中 和也*; 瀬古 典明

日本イオン交換学会誌, 25(4), p.248 - 251, 2014/11

An adsorbent for Scandium (Sc) recovery was developed with radiation-induced graft polymerization of phosphoric acids that have a high affinity for Sc onto polyethylene fabrics. The adsorption performance of Sc was evaluated with the Sc adsorption equipment, consisting of 155 mm internal diameter columns and a pump that were set up near Yukawa River in Kusatsu town. To achieve a practical use of Sc recovery, the adsorbent requires repeated use with maintaining its efficiency in terms of cost reduction. So, the reusability of the adsorbent was investigated by repeating adsorption and elution. The breakthrough curves of Sc adsorption showed similar behavior in all tests. The adsorbed Sc from the 19th adsorption test was 56 mg, which was comparable capacity to the average amount of the adsorbed Sc during the 19 tests. These results indicated that the adsorbent was used more than 19 times with maintaining high adsorption performance of Sc.

論文

Safe disassembly and storage of radioactive components of JT-60U torus

池田 佳隆; 岡野 文範; 花田 磨砂也; 逆井 章; 久保 博孝; 秋野 昇; 千葉 真一; 市毛 尚志; 神永 敦嗣; 清野 公広; et al.

Fusion Engineering and Design, 89(9-10), p.2018 - 2023, 2014/10

 被引用回数:2 パーセンタイル:16.31(Nuclear Science & Technology)

JT-60U本体の解体は、18年間の重水素運転の後、2009年から開始し、2012年10月に終了した。JT-60本体は電磁力に耐えるため複雑で溶接構造を有しており、機器は放射化している。本解体作業は、日本で初めての放射化した核融合装置の解体であり、注意深く実施された。約3年間で、約41,000人日の作業を行い、解体品総数は約13000個、総重量は5400トンに達した。全ての解体品は線量当量率等の測定を行っており、ほとんどの解体品は、将来、クリアランス検認を行えば、非放射化物となると期待できる。この解体が終了し、JT-60SAの組立が2013年1月から開始した。

論文

Optimization of grafted fibrous polymer as a solid basic catalyst for biodiesel fuel production

植木 悠二; 佐伯 誠一; 柴田 卓弥; 保科 宏行; 笠井 昇; 瀬古 典明

International Journal of Organic Chemistry, 4(2), p.91 - 105, 2014/06

第4級アミン基を有する繊維状グラフト重合体は、高性能なバイオディーゼル燃料(BDF)製造用触媒として機能する。本研究では、効率的なBDF製造を可能とする繊維状グラフト重合体、及び、エステル交換反応条件の最適化を実施した。触媒性能は、トリグリセリド(TG)とエタノール(EtOH)とのバッチ式エステル交換反応により評価した。触媒に導入する最適アミノ基はトリメチルアミンであり、最適グラフト率は170%であった。エステル交換反応における各要素の最適条件を検討した結果、アミン基導入量は0.8mmol、反応温度は80$$^{circ}$$C、TGとEtOHの混合比率は1:200、アルコールは1-ペンタノールでることを見出した。また、本触媒は天然油脂を出発原料とするBDF製造にも適用可能であった。更に、有機酸処理、アルカリ処理、アルコール処理を順次実施することにより、失活した触媒の活性を初期値まで回復させることに成功した。

報告書

放射線グラフト重合装置を用いたセシウム吸着材の作製とフィールド試験

笠井 昇; 岩撫 暁生; 植木 悠二; 佐伯 誠一; 保科 宏行; 瀬古 典明

JAEA-Technology 2013-046, 25 Pages, 2014/02

JAEA-Technology-2013-046.pdf:9.63MB

放射線グラフト重合法を適用して、セシウムに対して親和性が高い、リンモリブデン酸アンモニウムを担持した吸着材を開発した。実験室レベルで最適化した吸着材の作製条件をもとに150倍程度スケールアップしたベンチスケール規模の重合装置により、実験室規模の1,000倍量に相当する吸着材を作製し、実験室で作製したものと性能を比較評価した。また、作製した吸着材を用いて環境水中に溶存している放射性セシウムの吸着性能評価を福島県内でフィールド試験により行った。重合装置により得られた吸着材は、1ppmの安定性セシウムの水溶液を用いた吸着試験で、90%以上の吸着率を示した。また、吸着材を筒状のカラムに充填した吸着容量評価試験より、吸着材体積の3,000倍量の汚染水中のセシウムを吸着できることが分かった。さらに、福島県内で実施したフィールド試験では、水中に溶存する放射性セシウムを検出限界値以下まで除去できることを明らかにした。

論文

Adsorbent for arsenic(V) removal synthesized by radiation-induced graft polymerization onto nonwoven cotton fabric

保科 宏行; 高橋 牧克*; 笠井 昇; 瀬古 典明

International Journal of Organic Chemistry, 2(3), p.173 - 177, 2012/09

A fibrous adsorbent for arsenic (As) removal was synthesized with nonwoven cotton fabric as a trunk polymer. Phosphoric acid monomer was reacted by radiation-induced graft polymerization onto nonwoven cotton fabric. The degree of grafting of 130% was obtained at irradiation dose of 20 kGy with 5% of monomer solution for 2 hours reaction time at 40$$^{circ}$$C reaction temperature. After the grafted material was contacted with 10 mmol/L of zirconium (Zr) solution at pH1, 0.38 mmol/g of Zr as a functional group was loaded on the grafted phosphoric units for As(V) removal. The resulting adsorbent was evaluated by column mode adsorption with 1 mg/L of As(V) solution at various pH with space velocity 200 h$$^{-1}$$. The maximum capacity of As(V) adsorption was 0.1 mmol/g at pH2.

論文

Hybrid grafted ion exchanger for decontamination of radioactive cesium in Fukushima Prefecture and other contaminated areas

岩撫 暁生; 笠井 昇; 保科 宏行; 植木 悠二; 佐伯 誠一; 瀬古 典明

Journal of Radioanalytical and Nuclear Chemistry, 293(2), p.703 - 709, 2012/08

 被引用回数:35 パーセンタイル:91.99(Chemistry, Analytical)

放射線グラフト重合法を用いて、モリブデン酸アンモニウムとアクリロニトリルをポリエチレン製不織布に導入し、福島県地域に飛散したセシウムを除去するための吸着材を開発した。作製したセシウム吸着材のセシウム除去能をバッチ法とカラム法にて評価した。バッチ法ではセシウム濃度を1ppmに調製した純水,酸性溶液、及び海水中からセシウムをそれぞれ90, 87、及び64%除去することができた。カラム試験では、セシウム吸着材を直径7mm,高さ5mmに充填したカラムに1ppmのセシウム溶液を空間速度300h$$^{-1}$$の速度で通液し、流出液中のセシウム濃度を定量した。流出液中に供給液の1%の濃度のセシウムが検出された時点である破過点(C/C$$_{0}$$=0.01)における吸着容量は吸着材1kgあたり54gであった。福島県相馬郡飯舘村におけるセシウム吸着材のフィールド試験では、直径4cmのカラムにセシウム吸着材を3.8cmの高さまで充填し、放射性セシウムを含むため池水を通液し、水溶性の放射性セシウムを検出限界下まで除去できることができた。

論文

Synthesis of arsenic graft adsorbents in pilot scale

保科 宏行; 笠井 昇; 柴田 卓弥*; 明田川 康*; 高橋 牧克*; 吉井 明央*; 角田 安彦*; 瀬古 典明

Radiation Physics and Chemistry, 81(8), p.1033 - 1035, 2012/08

 被引用回数:4 パーセンタイル:31.65(Chemistry, Physical)

The zirconium (Zr(IV))-type adsorbent for As(V) removal was synthesized by radiation-induced graft polymerization with phosphoric monomer and the subsequent chemical modification with Zr(IV) by loading on phosphoric units. The Zr(IV)-type adsorbent can rapidly remove As(V) to low concentration. In order to apply for a large amount of water treatment, it is necessary to construct of synthesis method in pilot scale. Synthesis method of graft adsorbent in pilot scale was investigated by setting up the equipment which was composed of reaction tanks, washing tank and pump. The equipment can produce the adsorbent which is maximum 0.3 $$times$$ 20 m size in one batch graft reaction. To evaluate the optimum condition in this equipment, it was required the optimization of several condition such absorbed dose, monomer concentration, reaction temperature and reaction time. A nonwoven cotton fabric as a trunk polymer was irradiated, then it was placed into the reaction tank with the deaerated monomer solution. The components of the monomer was phosphoric acid mono- (50%) and di- (50%) ethyl methacrylate ester. As a result, the degree of grafting of 150% was obtained at absorbed dose of 20 kGy with 5% monomer solution mixed by deionized water for 2 hours at 40 $$^{circ}$$C. Finally after loaded of Zr(IV) on grafted nonwoven fabric, As(V) adsorbent was achieved in pilot scale.

論文

Current status of a new polarized neutron reflectometer at the intense pulsed neutron source of the Materials and Life Science Experimental Facility (MLF) of J-PARC

武田 全康; 山崎 大; 曽山 和彦; 丸山 龍治; 林田 洋寿; 朝岡 秀人; 山崎 竜也; 久保田 正人; 相澤 一也; 新井 正敏; et al.

Chinese Journal of Physics, 50(2), p.161 - 170, 2012/04

The construction of a new polarized neutron reflectometer is now in progress at the Materials and Life Science Experimental Facility (MLF) of the Japan Proton Accelerator Research Complex (J-PARC). MLF has the world's brightest pulsed neutron and muon sources (JSNS and MUSE). The user program of MLF has been already started in 2008, and now nine neutron and two muon spectrometers are in operation. Installation of the new reflectometer was expected to be completed in March 2011. However, the construction was interrupted by the massive earthquake hitting northeast Japan, including Tokai-mura where J-PARC is located. We expect to restart the user program of the new polarized neutron reflectometer at the beginning of next year (2012).

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