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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:1 パーセンタイル:38.14(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:5 パーセンタイル:23.48(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

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

Evaluation of the scandium affinity under the iron coexistence using radiation grafted adsorbents

林 菜月*; 保科 宏行; 天田 春代; 山延 健*; 瀬古 典明

日本イオン交換学会誌, 25(4), p.105 - 108, 2014/11

A fibrous phosphoric acid adsorbents for scandium were synthesized by radiation graft polymerization of glycidyl methacrylate (GMA), subsequent chemical modification, and direct grafting with a phosphoric monomer having both vinyl and phosphoric groups onto a polypropylene coated by polyethylene nonwoven fabric. The resultant grafted fibrous phosphoric acid adsorbent (HMP-g) having long side grafted chains has high affinity for scandium (Sc) ions even under the coexistence with Fe ion. The breakthrough capacity for Sc of 0.5 ppm with Fe coexistence was 10.9 mol-Sc per kg-adsorbent for the GMA derivative phosphoric adsorbent, and 17.8 mol-Sc per kg-adsorbent for HMP-g, respectively.

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

A New eco-friendly synthesis method for arsenic adsorbent

天田 春代; 高橋 牧克*; 保科 宏行; 瀬古 典明

日本イオン交換学会誌, 25(4), p.109 - 113, 2014/11

A large amount of arsenic waste solution which was dissolved in neutral aqueous media, was generated from the manufacturing process of gallium arsenide component in semiconductor industry. As for arsenic removal, an adsorbent was developed by radiation graft polymerization and subsequent chemical modification with N-methyl-D-glucamine (NMDG) as a functional group. Furthermore, the grafting and the modification were carried out using water based solvent instead of organic solvent in view of an environmental emission and a working environment. The solvents were comprised of water and surfactant, and the adsorption performances compared with a conventional method synthesized in 1,4-dioxane of organic solvent. Total amount of arsenic for arsenic(III) and arsenic(V) at pH 6.5 were 3.2 times and 2.1 times higher than our previous fibrous adsorbent. From the pH dependency studies, the developed grafted adsorbent gave high removal ratio in a neutral media area for both arsenic species. Breakthrough capacities in the column mode tests for arsenic(III) and arsenic(V) were 0.3 and 18 mg/g at pH 6.5, respectively.

論文

Synthesis of highly-selective fibrous adsorbent by introducing 2-ethylhexyl hydrogen-2-ethylhexylphosphonate for scandium adsorption

保科 宏行; 植木 悠二; 佐伯 誠一; 瀬古 典明

International Journal of Organic Chemistry, 4(3), p.195 - 200, 2014/09

2-Ethylhexyl hydrogen-2-ethylhexylphosphonate (EHEP) is commonly used as a metal extractant because it has a particular affinity for rare-earth metals like Scandium (Sc). To develop a highly-selective polymeric adsorbent of Sc(III), EHEP was introduced as a functional group onto a polyethylene fabric with radiation-induced graft polymerization (RIGP). The adsorption performances for Sc(III) were evaluated in aqueous solutions containing Sc(III) and Fe(III) by a column test. The adsorption capacities of Sc(III) and Fe(III) until the bed volume reached 5000 were 5.22 and 0.12 mg/g, respectively. The adsorbents showed 44 times higher Sc(III) adsorption capacity than that of Fe(III). These results indicated that the grafted adsorbent containing EHEP had an extremely high selectivity for Sc(III) adsorption.

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

A Novel avenue to gold nanostructured microtubes using functionalized fiber as the ligand, the reductant, and the template

Ma, H.*; Chi, H.*; Wu, J.*; Wang, M.*; Li, J.*; 保科 宏行; 佐伯 誠一; 瀬古 典明

Applied Materials & Interfaces, 5(17), p.8761 - 8765, 2013/09

Gold nanostructured microtubes (AuNMTs) are prepared using a tertiary amine group-functionalized polyethylene (PE)-coated polypropylene (PP) nonwoven fabric as a ligand, a reductant, and a template, which takes advantage of the different radiation effects of PE and PP. The Au(III) ions are absorbed and reduced only in the PE layer to form the aggregation of gold nanoparticles; thus, AuNMTs are obtained after the calcination.

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:21 パーセンタイル:8.06(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:1 パーセンタイル:85.4(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

Preparation of metal adsorbent from poly(methyl acrylate)-grafted-cassava starch via $$gamma$$ irradiation

Suwanmala, P.*; Hemvichian, K.*; 保科 宏行; Srinuttrakul, W.*; 瀬古 典明

Radiation Physics and Chemistry, 81(8), p.982 - 985, 2012/08

 被引用回数:10 パーセンタイル:25.58(Chemistry, Physical)

Metal adsorbent containing hydroxamic acid groups was successfully synthesized by radiation-induced graft copolymerization of methylacrylate onto cassava starch. The optimum conditions for grafting were studied in terms of % degree of grafting (Dg). Conversion of the ester groups present in poly(methyl acrylate)-grafted-cassava starch copolymer into hydroxamic acid was carried out by treatment with hydroxylamine in the presence of alkaline solution. The adsorbent of 191%Dg had total adsorption capacities of 2.6, 1.5, 1.4, 1.2 and 1.6 mmol/g-adsorbent for Cd$$^{2+}$$, Al$$^{3+}$$, UO$$_2^{2+}$$, V$$^{5+}$$, and Pb$$^{2+}$$, respectively, in the batch mode adsorption.

論文

Study and optimization on graft polymerization under normal pressure and air atmospheric conditions, and its application to metal adsorbent

植木 悠二; Dafader, N. C.*; 保科 宏行; 瀬古 典明; 玉田 正男

Radiation Physics and Chemistry, 81(7), p.889 - 898, 2012/07

 被引用回数:4 パーセンタイル:55.75(Chemistry, Physical)

By finding optimum grafting conditions, radiation-induced graft polymerization of glycidyl methacrylate (GMA) onto non-woven polyethylene (NWPE) fabric was achieved under normal pressure and air atmospheric conditions, even when a polyethylene bottle was used as a reactor instead of unique apparatus such as glass ampoules or vacuum lines. The optimum grafting conditions in this paper were as follows; the pre-irradiation dose was more than 50 kGy, the volume ratio of GMA-emulsion to air was 50:1 or less, and the dissolved oxygen concentration in GMA-emulsion during grafting was below 2.0 mg/L, respectively. Under these grafting conditions, the grafting yield was controlled up to 362%. The prepared GMA-grafted NWPE (GMA-g-NWPE) fabric was modified with a phosphoric acid to obtain a fibrous metal adsorbent. In the column-mode adsorption tests of Pb(II), the adsorption performance of the fibrous metal adsorbent was not essentially dependent on the flow rate of the feed. The breakthrough points of 200, 500, and 1000 h$$^{-1}$$ in space velocity were 483, 477 and 462 bed volumes, and the breakthrough capacities of the three flow rates were 1.16, 1.15 and 1.16 mmol-Pb(II)/g-adsorbent, respectively.

論文

Development of anion adsorbent for industry application based on biodegradable trunk material

笠井 昇; 保科 宏行; 瀬古 典明; 柴田 卓弥*; 高橋 牧克*

JAEA-Review 2011-043, JAEA Takasaki Annual Report 2010, P. 46, 2012/01

本研究は、有害物質が含まれる廃坑廃水や産業排水によって生じる水質汚染の一因となっているヒ素などの水中溶存アニオン系の有害物質を水質基準値以下まで浄化可能な吸着材を植物由来の生分解性素材を用いて創製し、実用化を目指すものである。本報告では、パイロット規模における吸着材の合成条件を確立するために製作したグラフト重合装置の特性試験結果及び実験室規模のビーカースケールで最適化したグラフト吸着材の合成条件を適用して大量合成を行った結果について報告する。幅30cm,長さ7mのセルロース基材を巻物状にしてグラフト重合し、得られた吸着材の吸着特性を調べた結果、ビーカースケールで作製した吸着材の性能と同等であり、巻物の長さ方向に対して、吸着率の分布は10%程度であり、均一な吸着材が得られた。

論文

Synthesis of amine-type adsorbents with emulsion graft polymerization of 4-hydroxybutyl acrylate glycidylether

Ma, H.; 森田 和明*; 保科 宏行; 瀬古 典明

Materials Sciences and Applications, 2(7), p.777 - 785, 2011/07

A pre-irradiation method was used for emulsion graft polymerization of 4-hydroxybutyl acrylate glycidylether (4-HB) onto polyethylene/polypropylene (PE/PP) nonwoven fabric. The degree of grafting (D$$_{rm g}$$) which can be calculated by weight increment was determined as a function of reaction time, irradiation dose, and monomer concentration. After 30 kGy irradiation, with 4-HB concentration of 5%, surfactant Span 20 of 0.5% at 40$$^{circ}$$C for 2 h, the trunk polymer was made grafted at a D$$_{rm g}$$ of 135%. 4-HB-grafted PE/PP nonwoven fabric was modified by ethylenediamine (EDA) in isopropyl alcohol (IPA) as a solvent at 60$$^{circ}$$C. The removal ratio from the EDA modified adsorbent of the metal ions is in the order of Cu$$^{2+}$$ $$>$$ Pb$$^{2+}$$ $$>$$ Zn$$^{2+}$$ $$>$$ Ni$$^{2+}$$ $$>$$ Li$$^{+}$$. Compared with glycidyl methacrylate (GMA) which is a typical functional monomer for graft polymerization, 4-HB-grafted adsorbent exhibited not only better mechanical property but also higher adsorption capacity of Cu$$^{2+}$$ and Pb$$^{2+}$$.

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