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Analysis of gadolinium oxide using microwave-enhanced fiber-coupled micro-laser-induced breakdown spectroscopy

池田 裕二*; Soriano, J. K.*; 大場 弘則; 若井田 育夫

Scientific Reports (Internet), 13, p.4828_1 - 4828_9, 2023/03

We report on the analysis of pure Gd oxide and its detection when mixed in surrogate nuclear debris using microwave-enhanced fiber-coupled micro-laser-induced breakdown spectroscopy. The target application is remote analysis of nuclear debris containing U inside the Fukushima Daiichi Nuclear Power Station. The surrogate nuclear debris used in this study contained Gd, Ce, Zr and Fe. The sample was ablated by microchip-laser under atmospheric pressure conditions while a helical antenna propagated 2.45 GHz 1.0 kW microwaves for 1.0 ms into the laser ablation plume. The results showed that microwave-induced plasma expansion led to enhanced emission signals of Gd I, Zr I, Fe I, Ce I, and Ce II. Microwave irradiation enhanced the standard deviations of the Gd and Ce emissions and lowered the detection limit of Gd by 60%.


Emulsification of low viscosity oil in alkali-activated materials

Reeb, C.*; Davy, C. A.*; Pierlot, C.*; Bertin, M.*; Cantarel, V.; Lambertin, D.*

Cement and Concrete Research, 162, p.106963_1 - 106963_16, 2022/12

 被引用回数:1 パーセンタイル:41.57(Construction & Building Technology)

Significant amounts of low viscosity mineral oil (20 %vol) are successfully immobilized in alkali-activated materials (AAM), either based on metakaolin or blast furnace slag. Surfactants are required to stabilize of the oil emulsion. Visual observation, torque measurement and rheology evidence two distinct groups of surfactants. One group contributes to structuring the oil/AAM fresh mix, with greater torque and viscosity than without surfactant; the other includes non-structuring surfactants, without change in torque or viscosity. Each group depends on the AAM considered. Whatever the AAM and the surfactant, the interfacial tension between oil/activating solution and the oil droplet size decrease significantly. Therefore, although contributing to stabilize the emulsion, interfacial tension alone does not explain the two distinct behaviors. Characterization of diluted ternary suspensions (solid particles-oil-AS) relates the structuring effect to interactions between oil and solid particles, through the surfactant polar head groups and non-polar hydrocarbon tails. An original mechanism explaining structuration is discussed.


被災地探査や原子力発電所建屋内情報収集のための半自律ロボットを用いたセマンティックサーベイマップ生成システムの開発(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; 東京工芸大学*

JAEA-Review 2022-011, 80 Pages, 2022/07




Geopolymer and ordinary Portland cement interface analyzed by micro-Raman and SEM

Cantarel, V.; 山岸 功

Journal of Nuclear Science and Technology, 59(7), p.888 - 897, 2022/07

 被引用回数:1 パーセンタイル:0.01(Nuclear Science & Technology)

Geopolymers are a class of material that could potentially be used for sealing and repair of damaged concrete structures. This application is important for both decommissioning activities and standard industrial applications. The purpose of this article is to investigate the interface between ordinary Portland cement and geopolymer. The surface microstructure of the cement is investigated by SEM, EDX, and micro-Raman after embedding in geopolymer or immersion in the activation solution of a geopolymer for various durations. It is found that immersion in the solution induces a dendritic carbonation profile into the cement structure following the CSH gel. On the contrary, embedding in the geopolymer creates a dense, impermeable interface with a thickness of a few micrometers. This interface is found to be dense and brittle and it decreases the permeability of the surface, preventing the penetration of silicates into the cement structure. However, this brittle interface is sensitive to dehydration and can rupture under intense drying. This phenomenon can be utilized to separate the geopolymer and cement but is concerning if the integrity of the material must be guaranteed under extreme conditions.


Evolution of the reaction and alteration of granite with Ordinary Portland cement leachates; Sequential flow experiments and reactive transport modelling

Bateman, K.*; 村山 翔太*; 花町 優次*; Wilson, J.*; 瀬田 孝将*; 天野 由記; 久保田 満*; 大内 祐司*; 舘 幸男

Minerals (Internet), 12(7), p.883_1 - 883_20, 2022/07

 被引用回数:0 パーセンタイル:0.02(Geochemistry & Geophysics)

The construction of a repository for geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository and the extensive use of cement will result in the development of a highly alkaline porewater, pH $$>$$ 12.5; this fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially high [Na] and [K], evolving to a Ca-rich fluid, and finally returning to the groundwater composition. This evolving chemistry will affect the long-term performance of the repository, altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction, as well as the formation and persistence of secondary mineral phases within a granite, comparing data from sequential flow experiments with the results of reactive transport modelling. The reaction of the granite with the cement leachates resulted in small changes in pH and the precipitation of calcium aluminum silicate hydrate (C-(A-)S-H) phases of varying compositions, of greatest abundance with the Ca-rich fluid. As the system evolved, secondary C-(A-)S-H phases re-dissolved, partly replaced by zeolites. This general sequence was successfully simulated using reactive transport modelling.


J-PARCにおける加速器駆動核変換システム(ADS)の研究開発,4; 陽子ビーム技術とニュートロニクス

明午 伸一郎; 中野 敬太; 岩元 大樹

プラズマ・核融合学会誌, 98(5), p.216 - 221, 2022/05




中野 敬太; 岩元 大樹; 西原 健司; 明午 伸一郎; 菅原 隆徳; 岩元 洋介; 竹下 隼人*; 前川 藤夫

JAEA-Research 2021-018, 41 Pages, 2022/03


加速器駆動核変換システム(ADS: Accelerator-Driven System)の構成要素の一つであるビーム窓の核特性を粒子・重イオン輸送計算コードPHITS及び誘導放射能解析コードDCHAIN-PHITSを用いて評価した。本研究では日本原子力研究開発機構が提案するADSの運転時にビーム窓内部に生成される水素やヘリウム等の量、高エネルギー粒子により引き起こされるビーム窓材の原子弾き出し数、ビーム窓内部の発熱量及び分布を導出した。また、中性子源標的及び冷却材として用いられる鉛ビスマス共晶合金(LBE)中の生成核種、発熱密度及び放射能分布を求めた。ビーム窓解析の結果、300日間のADSの運転によりビーム窓中に最大で約12500appmのH及び1800appmのHeの生成と62.1DPAの損傷が発生することが判明した。一方で、ビーム窓内の最大発熱量は374W/cm$$^3$$であった。LBEの解析では、$$^{206}$$Biや$$^{210}$$Poが崩壊熱及び放射能の支配的な核種であることが判明した。さらに、陽子ビームによるLBE中の発熱はビーム窓下流5cm付近が最大であり、945W/cm$$^3$$であることがわかった。


Development of JAEA sorption database (JAEA-SDB); Update of sorption/QA data in FY2021

杉浦 佑樹; 陶山 忠宏*; 舘 幸男

JAEA-Data/Code 2021-017, 58 Pages, 2022/03




Dynamic accommodation of internal stress and selection of crystallographic orientation relationship in pearlite

雨宮 雄太郎*; 中田 伸生*; 諸岡 聡; 小坂 誠*; 加藤 雅治*

ISIJ International, 62(2), p.282 - 290, 2022/02

 被引用回数:1 パーセンタイル:44.11(Metallurgy & Metallurgical Engineering)

To gain a deeper understanding of the dynamic accommodation mechanism of the internal stress in pearlite originating from the lattice misfit between ferrite and cementite phases, the lattice parameter ratios of cementite, b$$theta$$/a$$theta$$ and c$$theta$$/a$$theta$$, were locally analyzed in detail using the electron backscatter diffraction (EBSD) technique. The EBSD analysis revealed that the lattice parameter ratios of the cementite lamellae clearly differed from those of the spheroidized cementite particles, indicating that pearlite has a certain amount of internal stress as long as it maintains a lamellar structure. The internal stress in pearlite gradually decreased during the isothermal holding at 923 K after the pearlitic transformation due to the interfacial atomic diffusion of Fe atoms. However, a comparison with the theoretical values obtained from the Pitsch-Petch orientation relationship revealed that a large amount of internal stress had been already accommodated during the pearlitic transformation by the introduction of misfit dislocations and structural ledges on ferrite/cementite lamellar interfaces, i.e., the internal stress of pearlite is dynamically reduced by two different processes; built-in accommodation upon pearlitic transformation and additional time-dependent relaxation after pearlitic transformation. On the other hand, the analysis of the EBSD and neutron diffraction results yielded intriguingly different lattice parameters of cementite, indicating that various crystallographic orientation relationships between ferrite and cementite coexist in pearlite. Furthermore, the elastic strain energy analysis suggests that the invariant-line criterion on the ferrite/cementite interface plays an important role for the selection of orientation relationships in pearlite.


Decrease of radionuclide sorption in hydrated cement systems by organic ligands; Comparative evaluation using experimental data and thermodynamic calculations for ISA/EDTA-actinide-cement systems

Ochs, M.*; Dolder, F.*; 舘 幸男

Applied Geochemistry, 136, p.105161_1 - 105161_11, 2022/01

 被引用回数:3 パーセンタイル:82.95(Geochemistry & Geophysics)



Structural characterization by X-ray analytical techniques of calcium aluminate cement modified with sodium polyphosphate containing cesium chloride

高畠 容子; 渡部 創; 入澤 啓太; 塩飽 秀啓; 渡部 雅之

Journal of Nuclear Materials, 556, p.153170_1 - 153170_7, 2021/12

 被引用回数:1 パーセンタイル:25.87(Materials Science, Multidisciplinary)

The long-time experimental activities on pyroprocessing have generated waste eutectic salts contaminated with nuclear materials. After reprocessing tests, waste salts should be appropriately treated, with a focus on Cl disposal considering its corrosive nature. It is important to construct Cl confinement for the waste salts. Chlorapatite (Ca$$_{10}$$(PO$$_{4}$$)$$_{6}$$Cl$$_{2}$$) has great potential for Cl confinement due to Ca and P. The chemical reactivity of Cl will be drastically reduced if chlorapatite can be synthesized in calcium aluminate cement modified with sodium polyphosphate (CAP) containing CsCl. This study confirms the chemical state of Cl and metal elements in the cement by XRD, XPS, and XANES in the CAP containing CsCl. The analyses results suggest the existence of the Ca-Cl-Cs and Al-Cl-Cs bonds in CAP containing CsCl. The formation of the chemical bonds of Cl with metal elements might be one of important factors for the chlorapatite formation from the CAP containing CsCl.


Evolution of the reaction and alteration of mudstone with ordinary Portland cement leachates; Sequential flow experiments and reactive-transport modelling

Bateman, K.; 村山 翔太*; 花町 優次*; Wilson, J.*; 瀬田 孝将*; 天野 由記; 久保田 満*; 大内 祐司*; 舘 幸男

Minerals (Internet), 11(9), p.1026_1 - 1026_23, 2021/09

 被引用回数:2 パーセンタイル:36.87(Geochemistry & Geophysics)

The construction of a repository for geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository and the extensive use of cement will result in the development of a highly alkaline porewater, pH $$>$$ 12.5. This fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially high [Na] and [K], evolving to a Ca-rich fluid and finally returning to the groundwater composition. This evolving chemistry will affect the long-term performance of the repository altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction; the formation and persistence of secondary mineral phases within an argillaceous mudstone, comparing both data from sequential flow experiments with the results of reactive transport modeling. The reaction of the mudstone with the cement leachates resulted in small changes in pH but the precipitation of calcium aluminium silicate hydrate (C-A-S-H) phases of varying compositions. With the change to the groundwater secondary C-(A-)S-H phases re-dissolved being replaced by secondary carbonates. This general sequence was successfully simulated by the reactive transport model simulations.


Hydrogen permeation property of bulk cementite

足立 望*; 上野 春喜*; 尾上 勝彦*; 諸岡 聡; 戸高 義一*

ISIJ International, 61(8), p.2320 - 2322, 2021/08

 被引用回数:1 パーセンタイル:14.34(Metallurgy & Metallurgical Engineering)

This study investigated the hydrogen permeation property of cementite by fabricating bulk cementite sample using the process combining the mechanical ball milling and subsequent pulse current sintering. The bulk cementite sample having a 96 vol% of cementite was successfully fabricated. The prepared bulk cementite showed no signal of hydrogen permeation during the 3.5 day of electrochemical hydrogen permeation test. The morphology of blister formed in the sample indicated that diffusion coefficient of hydrogen in cementite is very small.


The Impact of cement on argillaceous rocks in radioactive waste disposal systems; A Review focusing on key processes and remaining issues

Wilson, J.*; Bateman, K.; 舘 幸男

Applied Geochemistry, 130, p.104979_1 - 104979_19, 2021/07

 被引用回数:8 パーセンタイル:63.18(Geochemistry & Geophysics)



Reaction and alteration of mudstone with Ordinary Portland Cement and Low Alkali Cement pore fluids

Bateman, K.; 天野 由記; 久保田 満*; 大内 祐司*; 舘 幸男

Minerals (Internet), 11(6), p.588_1 - 588_19, 2021/06

 被引用回数:4 パーセンタイル:63.17(Geochemistry & Geophysics)

The alkaline fluid arising from the cement-based materials will react with host rock to form a chemically disturbed zone around the geological disposal repository. To understand how these conditions may evolve, a series of batch and flow experiments were conducted with Horonobe mudstone and fluids representative of the alkaline leachates expected from both Ordinary Portland Cement (OPC) and Low Alkali Cement (LAC) leachates. The impact of the LAC was more limited, compared to the OPC leachates. Ion exchange reactions had an impact initially but thereafter the reaction was dominated by primary mineral dissolution, and in the case of OPC leachates precipitation of secondary C-S-H phases. The flow experiments revealed that precipitation of the secondary phases was restricted to close to the initial contact zone of the fluids and mudstone. The experimental results demonstrate that a combination of both batch and flow-through experiments can provide the insights required for the understanding of the key geochemical interactions and the impact of transport, allowing the spatial as well as temporal evolution of the alkaline leachate / mudstone system to be determined.


被災地探査や原子力発電所建屋内情報収集のための半自律ロボットを用いたセマンティックサーベイマップ生成システムの開発(委託研究); 令和元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; 東京工芸大学*

JAEA-Review 2020-062, 47 Pages, 2021/01




最先端の研究開発,日本原子力研究開発機構,6; 廃止措置と廃棄物の処理処分を目指して,1; 低レベル放射性廃棄物の処理処分とウラン鉱山閉山措置に関する技術開発

辻 智之; 杉杖 典岳; 佐藤 史紀; 松島 怜達; 片岡 頌治; 岡田 翔太; 佐々木 紀樹; 井上 準也

日本原子力学会誌ATOMO$$Sigma$$, 62(11), p.658 - 663, 2020/11




中山 雅

JAEA-Data/Code 2020-009, 98 Pages, 2020/09


幌延深地層研究センターの地下施設において、原子力機構が開発した低アルカリ性セメント(Highly Fly-ash contained Silicafume Cement: HFSC)を用いた吹付けコンクリート(深度140m, 250m, 350m調査坑道)および覆工コンクリート(東立坑深度374m$$sim$$380m)の原位置施工試験を実施した。HFSCの周辺岩盤および地下水への影響を評価するため、原位置施工試験の実施箇所から定期的にコンクリートおよび岩石のコアを採取し、各種分析を実施した。また、140m調査坑道においては、普通ポルトランドセメント(OPC)の施工区間を設け、HFSCと同様の分析を行い、OPCとHFSCの影響の違いについて比較した。本データ集は、平成21年から平成30年にかけて、各深度からのコア試料に対して実施した分析結果について取りまとめたものである。


Continuous and discontinuous yielding behaviors in ferrite-cementite steels

Wang, Y.*; 友田 陽*; 大村 孝仁*; Gong, W.*; Harjo S.; 田中 雅彦*

Acta Materialia, 196, p.565 - 575, 2020/09

 被引用回数:25 パーセンタイル:90.28(Materials Science, Multidisciplinary)

The continuous and discontinuous yielding behaviors in ferrite-cementite steels were complementarily investigated via nano- and macroscale deformation examinations. The results obtained by electron microscopy, synchrotron X-ray, and neutron diffractions indicate that the ferrite-cementite interface of the heat-treated specimen is semi-coherent with a high internal stress field, whereas that of the recrystallized one is incoherent with a low internal stress field. Moreover, coherency strain, which depends on the total area of the ferrite-cementite interface, and thermal strain, which is governed by temperature, are the two factors that influence peak broadening. The nanoindentation tests revealed that the critical loads are significantly lower near the semi-coherent interface than those near the incoherent interface and the ferrite grain boundary; this suggests that dislocations are easily emitted from the semi-coherent interface.



青柳 和平; 櫻井 彰孝; 宮良 信勝; 杉田 裕

JAEA-Research 2020-004, 68 Pages, 2020/06



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