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Pd nanoparticles on the outer surface of microporous aluminosilicates for the direct alkylation of benzenes using alkanes

美崎 慧*; 三輪 寛子*; 伊藤 孝; 吉田 健文*; 長谷川 慎吾*; 中村 由紀奈*; 徳竹 駿太*; 高畠 萌*; 下村 浩一郎*; Chun, W.-J.*; et al.

ACS Catalysis, 13(18), p.12281 - 12287, 2023/09

The direct alkylation of benzenes with simple alkanes is one of the ideal processes for the production of alkylbenzenes. We demonstrated that Pd nanoparticles on the outer surface of H-ZSM-5 are efficient catalysts for direct alkylation. The reaction proceeds through the activation of an alkane on the acid sites present inside the zeolite pores. This process is followed by the nucleophilic addition of an arene to the activated alkane. The spillover of the abstracted hydrogen atoms from the acid sites to the Pd nanoparticles on the outer surface accelerates recombination to H$$_2$$. A maximum toluene conversion of 58.5% and selectivity of 95.6% for the alkylated products are achieved when toluene is reacted with $$n$$-heptane. ${it Para}$-selective alkylation is achieved, due to the effect of the pore size of H-ZSM-5. The $$mu^+$$SR study of muonium, a pseudo-isotope of hydrogen, in aluminosilicates suggested that the formation of atomic hydrogen is possible and its lifetime is in the sub-microsecond range or longer, which is long enough for chemical reactions.


Cavitation damage prediction in mercury target for pulsed spallation neutron source using Monte Carlo simulation

涌井 隆; 高岸 洋一*; 二川 正敏

Materials, 16(17), p.5830_1 - 5830_16, 2023/09

水銀ターゲット容器は、陽子ビームの入射に伴い、キャビテーション損傷を受けるため、キャビテーションバブルの位置や衝撃圧力分布の不確実さを考慮して、モンテカルロ・シミュレーションを用いたキャビテーション損傷を予測する手法を提案した。本手法では、個々のキャビテーション気泡の崩壊に起因する衝撃圧力の分布はガウス分布とし、衝撃圧力の最大値の確率密度分布は3種類の分布: デルタ関数、ガウス分布、ワイブル分布と仮定した。衝撃圧力の分布を記述する方程式の2つのパラメータについて、実験から得られたキャビテーション損傷の分布とシミュレーションから得られた累積塑性ひずみの分布を比較し、ベイズ最適化を使用して推定することができた。また、ワイブル分布を用いて得られた結果が、他の結果に比べて、実際のキャビテーションエロージョン現象を再現することが分かった。


A Predicted CRISPR-mediated symbiosis between uncultivated archaea

Esser, S. P.*; Rahlff, J.*; Zhao, W.*; Predl, M.*; Plewka, J.*; Sures, K.*; Wimmer, F.*; Lee, J.*; Adam, P. S.*; McGonigle, J.*; et al.

Nature Microbiology (Internet), 8(9), p.1619 - 1633, 2023/09


CRISPR-Cas systems defend prokaryotic cells from viruses, plasmids, and other mobile genetic elements. Capitalizing on multi-omics approaches, we show here that the CRISPR-Cas systems of uncultivated archaea also play an integral role in mitigating potentially detrimental interactions with episymbionts. A comprehensive analysis of CRISPR-Cas-based infection histories revealed that uncultivated deep-subsurface archaeal primary-producers defend themselves from archaeal episymbionts of the DPANN superphylum of archaea, some of which are known to fuse their membranes with their host. We show that host cells counter these attacks by deploying one of two CRISPR-Cas systems (type I-B and type III-A) to target and disrupt essential genes in the episymbiont. However, genome-scale modeling of metabolic interactions between two deep subsurface host-symbiont systems revealed that host cells also benefit from the symbionts via metabolic complementation. We speculate that populations of these uncultivated archaeal episymbionts are currently transitioning from a parasitic lifestyle to one of mutualism, as must have occurred in countless mutualistic systems known today. By expanding our analysis to thousands of archaeal genomes, we conclude that CRISPR-Cas mediated resistance to archaeal episymbiosis evolved independently in various archaeal lineages and may be a wide-spread evolutionary phenomenon.


Hierarchical Bayesian modeling to quantify fracture limit uncertainty of high-burnup advanced fuel cladding tubes under loss-of-coolant accident conditions

成川 隆文; 濱口 修輔*; 高田 孝*; 宇田川 豊

Nuclear Engineering and Design, 411, p.112443_1 - 112443_12, 2023/09


For realizing a highly reliable fracture limit evaluation of fuel cladding tubes during loss-of-coolant accidents (LOCAs) in light-water reactors, we developed a method to quantify the fracture limit uncertainty of high-burnup advanced fuel cladding tubes. This method employs a hierarchical Bayesian model that can quantify uncertainty even with limited experimental data. The fracture limit uncertainty was quantified as a probability using the amount of oxidation (Equivalent cladding reacted: ECR) and the initial hydrogen concentration (the hydrogen concentration in the fuel cladding tubes before the LOCA-simulated tests) as explanatory variables. We divided the regression coefficients of this model into a hierarchical structure with an overall average term common to all types of fuel cladding tubes and a term representing differences among various types of fuel cladding tubes. This hierarchical structure enabled us to quantify the fracture limit uncertainty through the effective use of prior knowledge and data, even for high-burnup advanced fuel cladding tubes with a small number of data points. The fracture limits representing a 5% fracture probability with 95% confidence of the high-burnup advanced fuel cladding tubes evaluated by the hierarchical Bayesian model were higher than 15% ECR for the initial hydrogen concentrations of up to 700-900 wtppm and restraint loads below 535 N. These fracture limits were comparable to the limit of the unirradiated Zircaloy-4 cladding tube, indicating that the burnup extension and use of the advanced fuel cladding tubes do not significantly lower the fracture limit of fuel cladding tubes. Further, we proposed a method to reduce the fracture limit uncertainty by using non-binary data, instead of the binary data, depending on the condition of the fuel cladding tube specimens after performing the LOCA-simulated test, thereby increasing the amount of information in the data.



外川 織彦; 外間 智規; 平岡 大和

JAEA-Review 2023-013, 48 Pages, 2023/08




Paleoclimatic controls on natural tracer profiles in biogenic sedimentary formations of the Horonobe area, Japan

Arthur, R.*; 笹本 広; Alt-Epping, P.*; 舘 幸男

Applied Geochemistry, 155, p.105707_1 - 105707_8, 2023/08

 被引用回数:0 パーセンタイル:0.01(Geochemistry & Geophysics)



Behavior of FeCrAl-ODS cladding tube under loss-of-coolant accident conditions

成川 隆文; 近藤 啓悦; 藤村 由希; 垣内 一雄; 宇田川 豊; 根本 義之

Journal of Nuclear Materials, 582, p.154467_1 - 154467_12, 2023/08

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

To evaluate the behavior of an oxide-dispersion-strengthened FeCrAl (FeCrAl-ODS) cladding tube under loss-of-coolant accident (LOCA) conditions of light-water reactors (LWRs), the following two laboratory-scale LOCA-simulated tests were performed: the burst and integral thermal shock tests. Four burst and three integral thermal shock tests were performed on unirradiated, stress-relieved FeCrAl-ODS cladding tube specimens, simulating ballooning and rupture, oxidation, and quenching, which were postulated during a LOCA. The burst temperature of the FeCrAl-ODS cladding tube was 200-300 K higher than that of the Zircaloy cladding tube, and the FeCrAl-ODS cladding tube's maximum circumferential strain was smaller than or equal to the Zircaloy-4 cladding tube. These results indicate that the FeCrAl-ODS cladding tube has higher strength at high temperatures than the conventional Zircaloy cladding tube. The FeCrAl-ODS cladding tube did not fracture after being subjected to an axial restraint load of $$sim$$5000 N, which is more than 10 times higher than the axial restraint load estimated for existing LWRs, during quenching, following isothermal oxidation at 1473 K for 1 h. The FeCrAl-ODS cladding tube was hardly oxidized during this isothermal oxidation condition. However, it melted after a short oxidation at 1673 K and fractured after abnormal oxidation at 1573 K for 1 h. Based on these results, the FeCrAl-ODS cladding tube should not fracture in the time range expected during LOCAs below 1473 K, where no melting or abnormal oxidation occurs.


Optimization of dissolved hydrogen concentration for mitigating corrosive conditions of pressurised water reactor primary coolant under irradiation, 2; Evaluation of electrochemical corrosion potential

端 邦樹; 塙 悟史; 知見 康弘; 内田 俊介; Lister, D. H.*

Journal of Nuclear Science and Technology, 60(8), p.867 - 880, 2023/08

 被引用回数:2 パーセンタイル:49.42(Nuclear Science & Technology)



Radiation imaging of a highly contaminated filter train inside Fukushima Daiichi Nuclear Power Station Unit 2 using an integrated Radiation Imaging System based on a Compton camera

佐藤 優樹; 寺阪 祐太

Journal of Nuclear Science and Technology, 60(8), p.1013 - 1026, 2023/08

 被引用回数:1 パーセンタイル:89.37(Nuclear Science & Technology)

The Fukushima Daiichi Nuclear Power Station (FDNPS) suffered a meltdown in the aftermath of the large tsunami caused by the Great East Japan Earthquake that occurred on 11 March 2011. A massive amount of radioactive substance was spread over a wide area both inside and outside the FDNPS site. In this study, we present an approach for visualizing a radioactive hotspot on a standby gas-treatment system filter train, a highly contaminated piece of equipment in the air-conditioning room of the Unit 2 reactor building of FDNPS, using radiation imaging based on a Compton camera. In addition to fixed-point measurements using only the Compton camera, data acquisition while moving using an integrated Radiation Imaging System (iRIS), which combines a Compton camera with a simultaneous localization and mapping device and a survey meter, enabled the three-dimensional visualization of the hotspot location on the filter train. In addition, we visualized the hotspot and quantitatively evaluated its radioactivity. Notably, the visualized hotspot location and estimated radioactivity value are consistent with the accident investigation report of the FDNPS. Finally, the extent to which the radioactivity increased the ambient dose equivalent rate in the surrounding environment was explored.


Reactor physics experiment on a graphite-moderated core to construct integral experiment database for HTGR

沖田 将一朗; 深谷 裕司; 左近 敦士*; 佐野 忠史*; 高橋 佳之*; 宇根崎 博信*

Nuclear Science and Engineering, 197(8), p.2251 - 2257, 2023/08

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

In this paper, integral experiments on a graphite-moderated core were conducted at the B-rack of the Kyoto University Criticality Assembly in order to develop an integral experiment database for the applicability of data assimilation techniques to the neutronic design of a high-temperature gas-cooled reactor. The calculation/experiment-1 (C/E-1)values for the $$k_{rm eff}$$ values at critical cores with the major nuclear data libraries, such as JENDL-4.0, JENDL-5, JEFF-3.2, ENDF/B-VII.1, and ENDF/B-VIII.0, were calculated for the core. Of these, the $$k_{rm eff}$$ values with JENDL-5 with thermal neutron scattering law data for 30% porous graphite showed the best agreement with experimental values within 0.02% accuracy.




JAEA-Evaluation 2023-001, 38 Pages, 2023/07




Data report of ROSA/LSTF experiment IB-HL-01; 17% hot leg intermediate break LOCA with totally-failed high pressure injection system

竹田 武司

JAEA-Data/Code 2023-007, 72 Pages, 2023/07


ROSA-V計画において、大型非定常実験装置(LSTF)を用いた実験(実験番号:IB-HL-01)が2009年11月19日に行われた。ROSA/LSTF IB-HL-01実験では、加圧水型原子炉(PWR)の加圧器サージラインの両端ギロチン破断による17%高温側配管中破断冷却材喪失事故を模擬した。このとき、高温側配管内面に接する様に、長いノズルを上向きに取り付けることにより破断口を模擬した。また、非常用炉心冷却系(ECCS)である高圧注入系の全故障と補助給水系の全故障を仮定した。実験では、比較的大きいサイズの破断が早い過渡現象を引き起こした。破断後一次系圧力が急激に低下し、蒸気発生器(SG)二次側圧力よりも低くなった。破断流は、破断直後に水単相から二相流に変化した。炉心露出は、ループシールクリアリング(LSC)前に、クロスオーバーレグの下降流側の水位低下と同時に開始した。低温側配管に注入されたECCSの蓄圧注入系(ACC)冷却水の蒸気凝縮により両ループのLSCが誘発された。LSC後の炉心水位の急速な回復により、全炉心はクエンチした。模擬燃料棒被覆管最高温度は、LSCとほぼ同時に検出された。ACC冷却水注入時、高速蒸気流による高温側配管からSG入口プレナムへの液体のエントレインメントにより、高温側配管とSG入口プレナムの水位が回復した。ECCSである低圧注入系の作動を通じた継続的な炉心冷却を確認後、実験を終了した。本報告書は、ROSA/LSTF IB-HL-01実験の手順、条件および実験で観察された主な結果をまとめたものである。


The Development of a Multiphysics Coupled Solver for Studying the Effect of Dynamic Heterogeneous Configuration on Particulate Debris Bed Criticality and Cooling Characteristics

Li, C.-Y.; Wang, K.*; 内堀 昭寛; 岡野 靖; Pellegrini, M.*; Erkan, N.*; 高田 孝*; 岡本 孝司*

Applied Sciences (Internet), 13(13), p.7705_1 - 7705_29, 2023/07


For a sodium-cooled fast reactor, the capability for stable cooling and avoiding re-criticality on the debris bed is essential for achieving in-vessel retention when severe accidents occur. However, an unexploited uncertainty still existed regarding the compound effect of the heterogeneous configuration and dynamic particle redistribution for the debris bed's criticality and cooling safety assessment. Therefore, this research aims to develop a numerical tool for investigating the effects of the different transformations of the heterogeneous configurations on the debris bed's criticality/cooling assessment. Based on the newly proposed methodology in this research, via integrating the Discrete Element Method (DEM) with Computational Fluid Dynamics (CFD) and Monte-Carlo-based Neutronics (MCN), the coupled CFD-DEM-MCN solver was constructed with the originally created interface to integrate two existing codes. The effects of the different bed configurations' transformations on the bed safety assessments were also quantitively confirmed, indicating that the effect of the particle-centralized fissile material had the dominant negative effect on the safety margin of avoiding re-criticality and particle re-melting accidents and had a more evident impact than the net bed-centralized effect. This coupled solver can serve to further assess the debris bed's safety via a multi-physics simulation approach, leading to safer SFR design concepts.


Impact of MOX fuel use in light-water reactors; Long-term radiological consequences of disposal of high-level waste in a geological repository

三成 映理子*; 樺沢 さつき; 三原 守弘; 牧野 仁史; 朝野 英一*; 中瀬 正彦*; 竹下 健二*

Journal of Nuclear Science and Technology, 60(7), p.793 - 803, 2023/07

 被引用回数:1 パーセンタイル:49.42(Nuclear Science & Technology)

As a series of studies to evaluate impact of mixed-oxide (MOX) fuel in light-water reactors (LWRs), post-closure long-term safety for various vitrified high-level radioactive waste (HLW) arising from the different fuel cycle intends to recycle Pu are examined. In this study, four fuel cycle scenarios with different ratio of spent MOX generated and two reprocessing options for each fuel cycle scenario are considered. One reprocessing option considers disposal of vitrified HLW generated separately from the reprocessing of spent UO$$_{2}$$ fuel and MOX fuel (separated HLW), and the other is blended vitrified UO$$_{2}$$-MOX HLW (blended HLW) generated during reprocessing whereby MOX spent fuel is diluted by UO$$_{2}$$ spent fuel. First, the radionuclide inventories of those vitrified HLWs are discussed. Next, radionuclide migration analyses for geological disposal of those vitrified HLWs are evaluated. It has revealed that the disposal of blended HLW will not have an adverse effect on the long-term radiological impact compared to separated HLW. Results of this study can be used as a basis for considering the blending option as a viable alternative approach in the future for managing MOX fuel used in light-water reactors.


Establishing an evaluation method for the aging phenomenon by physical force in fuel debris

鈴木 誠矢; 荒井 陽一; 岡村 信生; 渡部 雅之

Journal of Nuclear Science and Technology, 60(7), p.839 - 848, 2023/07

 被引用回数:0 パーセンタイル:0.02(Nuclear Science & Technology)



Radio-tellurium released into the environment during the complete oxidation of fuel cladding, containment venting and reactor building failure of the Fukushima accident

日高 昭秀; 川島 茂人*; 梶野 瑞王*

Journal of Nuclear Science and Technology, 60(7), p.743 - 758, 2023/07

 被引用回数:2 パーセンタイル:89.37(Nuclear Science & Technology)

福島事故時に放出された放射性物質量の推定は、原子炉の事故進展や環境影響の評価にとって不可欠である。そこで、ヨウ素,Csに次いで放出量が多いTeについて、単位放出量を想定したメソスケール気象モデル計算で得られた時間ごとの沈着量に基づいて沈着量分布を重み付けする、単位放出回帰推定法を用いて検討した。前回の検討では、この手法の適用性確認に主眼を置き、発生源について暫定的な結果を得ることができた。しかし、その後の検討で、放出があったと思われる期間の一部が放出推定期間から欠落していると、ソースターム計算全体に歪みが生じることが判明した。このため、本研究では、推定期間を延長し、主要な放出を全て含むように再計算を行った。その結果、これまで特定されなかった放出事象が明らかになり、炉内事象との対応も確認できた。また、炉心注水時のZr被覆管完全酸化による$$^{rm 129m}$$Te放出事象を考慮することにより、土壌汚染マップにおける$$^{rm 129m}$$Te/$$^{137}$$Cs比の地域依存性を説明することができた。さらに、本検討に基づき、WSPEEDI逆計算では予測できなかった3月11日夜,13日,14日早朝にヨウ素とCsの放出が増加した可能性を指摘した。


Local electronic structure of interstitial hydrogen in MgH$$_2$$ inferred from muon study

門野 良典*; 平石 雅俊*; 岡部 博孝*; 幸田 章宏*; 伊藤 孝

Journal of Physics; Condensed Matter, 35(28), p.285503_1 - 285503_13, 2023/07

Magnesium hydride has great potential as a solid hydrogen (H) storage material because of its high H storage capacity of 7.6 wt%. However, its slow hydrogenation and dehydrogenation kinetics and the high temperature of 300 $$^circ$$C required for decomposition are major obstacles to small-scale applications such as automobiles. The local electronic structure of interstitial H in MgH$$_2$$ is an important fundamental knowledge in solving this problem, which has been studied mainly based on density functional theory (DFT). However, few experimental studies have been performed to assess the results of DFT calculations. We have therefore introduced muon (Mu) as pseudo-H into MgH$$_2$$ and investigated the corresponding interstitial H states by analyzing their electronic and dynamical properties in detail. As a result, we observed multiple Mu states similar to those observed in wide-gap oxides, and found that their electronic states can be attributed to relaxed-excited states associated with donor/acceptor levels predicted by the recently proposed ambipolarity model. This provides an indirect support for the DFT calculations on which the model is based via the donor/acceptor levels. An important implication of the muon results for improved hydrogen kinetics is that dehydrogenation, serving as a reduction for hydrides, stabilises the interstitial H$$^-$$ state.


Spontaneous topological Hall effect induced by non-coplanar antiferromagnetic order in intercalated van der Waals materials

高木 寛貴*; 高木 里奈*; 見波 将*; 野本 拓也*; 大石 一城*; 鈴木 通人*; 柳 有起*; 平山 元昭*; Khanh, N.*; 軽部 皓介*; et al.

Nature Physics, 19(7), p.961 - 968, 2023/07

 被引用回数:0 パーセンタイル:0.01(Physics, Multidisciplinary)

In ferromagnets, electric current generally induces a transverse Hall voltage in proportion to the internal magnetization. This effect is frequently used for electrical readout of the spin up and down states. While these properties are usually not expected in antiferromagnets, recent theoretical studies predicted that non-coplanar antiferromagnetic order with finite scalar spin chirality - meaning a solid angle spanned by neighboring spins - can induce a large spontaneous Hall effect even without net magnetization or external magnetic field. This phenomenon, the spontaneous topological Hall effect, can potentially be used for the efficient electrical readout of the antiferromagnetic states, but it has not been experimentally verified due to a lack of appropriate materials hosting such magnetism. Here, we report the discovery of all-in-all-out type non-coplanar antiferromagnetic order in triangular lattice compounds CoTa$$_{3}$$S$$_{6}$$ and CoNb$$_{3}$$S$$_{6}$$. These compounds are reported to host unconventionally large spontaneous Hall effect despite their vanishingly small net magnetization, and our analysis reveals that it can be explained in terms of the topological Hall effect that originates from the fictitious magnetic field associated with scalar spin chirality. These results indicate that the scalar spin chirality mechanism offers a promising route to the realisation of giant spontaneous Hall response even in compensated antiferromagnets, and highlight intercalated van der Waals magnets as a promising quasi-two-dimensional material platform to enable various nontrivial ways of electrical reading and possible writing of non-coplanar antiferromagnetic domains.



石塚 悦男; Ho, H. Q.; 北川 堪大*; 福田 理仁*; 伊藤 諒*; 根本 将矢*; 楠木 捷斗*; 野村 拓朗*; 長瀬 颯太*; 橋本 温希*; et al.

JAEA-Technology 2023-013, 19 Pages, 2023/06





原子力科学研究部門 原子力科学研究所

JAEA-Review 2023-009, 165 Pages, 2023/06



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