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

https://doi.org/10.1021/acscatal.3c02309

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. A maximum toluene conversion of 58.5% and selectivity of 95.6% for the alkylated products are achieved when toluene is reacted with -heptane. -selective alkylation is achieved, due to the effect of the pore size of H-ZSM-5. The 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.

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

https://doi.org/10.1038/s41564-023-01439-2

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.

原子力災害時における車両の汚染状況と除染措置に関する調査と検討

外川 織彦; 外間 智規; 平岡 大和

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

JAEA-Review-2023-013.pdf:2.11MB

原子力災害時に大気へ放射性物質が放出された場合には、住民等の被ばくを低減するための防護措置として、自家用車やバス等の車両を利用して避難や一時移転が実施される。避難等を実施した住民等の汚染状況を確認するため避難退域時検査が行われるが、その迅速性を損なわないことが重要である。現状の検査では、車両の指定箇所検査をワイパー部とタイヤ側面で実施し、要員によるGMサーベイメータ等の表面汚染検査用測定器で検査することを基本としている。また、車両の迅速かつ効率的な検査実施のため、可搬型車両用ゲート型モニタの活用も計画されているところである。本報告書では、迅速かつ効率的な避難退域時検査に資するため、原子力災害時における車両の汚染状況と除染措置に関する調査を実施した。利用可能な関連文献や情報はごく少数であったが、当該文献等に記載された調査結果を目的に応じて抽出して整理するとともに、避難退域時検査の迅速かつ効率的な運用という観点からその調査結果について検討を行った。

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

https://doi.org/10.1016/j.jnucmat.2023.154467

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 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.

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

https://doi.org/10.1080/00223131.2022.2159894

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.

令和4年度計算科学技術研究実績評価報告

システム計算科学センター

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

JAEA-Evaluation-2023-001.pdf:1.04MB

システム計算科学センターでは、「国立研究開発法人日本原子力研究開発機構の中長期目標を達成するための計画(中長期計画)」に基づき、原子力分野における計算科学技術研究に関する研究開発を実施してきた。その計算科学技術研究の実績については、計算科学技術研究・評価委員会(以下「委員会」という。)により評価された。本報告は、システム計算科学センターにおいて実施された計算科学技術研究の、令和4年度における業務の実績及びそれらに対する委員会による評価結果をとり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

https://doi.org/10.3390/app13137705

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.

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

https://doi.org/10.1080/00223131.2022.2159559

福島第一原子力発電所の事故で発生した燃料デブリは、溶融した核燃料物質と原子炉の構造材等で構成された酸化物が多くを占めているため、環境温度の変化により岩石のように劣化する可能性が高い。燃料デブリは10年以上水冷されているが、季節や昼夜の温度変化の影響を少なからず受けていることから、燃料デブリの経年変化挙動を評価するためには環境温度の変化を考慮することが不可欠である。仮に燃料デブリの劣化が進んでいる場合、微粉化した放射性物質が冷却水中に溶出して取出し作業に影響を及ぼす可能性がある。本研究では、環境温度の繰り返し変化がクラックの発生に与える影響に着目して、燃料デブリの模擬体を用いた加速試験を実施した。その結果、クラックは温度変化を重ねることで増加することを確認し、燃料デブリの簿擬態は熱膨張と収縮による応力により脆化することが判明した。燃料デブリの物理学的な劣化挙動は岩石や鉱物に類似していることが確認され、模擬燃料デブリと環境のモデルでクラックの増加挙動を予測することが可能となった。

Local electronic structure of interstitial hydrogen in MgH 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

https://doi.org/10.1088/1361-648X/acccc7

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 C required for decomposition are major obstacles to small-scale applications such as automobiles. The local electronic structure of interstitial H in MgH 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 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.

2022年度夏期休暇実習報告

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

JAEA-Technology-2023-013.pdf:1.75MB

「HTTRに関する技術開発」をテーマとした2022年度夏期休暇実習において、5つの大学から8名が参加した。参加者は、原子力電池の検討、HTTR炉心の燃焼解析、Cf製造の検討、冷却機能喪失時の挙動解析、炉容器近傍の熱流動解析について実習した。実習後のアンケートでは、就業体験として有益であったこと、一部の学生においては自身の研究に役立ったこと、他の大学生との議論が良い経験となった等の感想があり、本実習は概ね良好な評価を得た。