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Research and development on membrane IS process for hydrogen production using solar heat

Odtsetseg, M.; 岩月 仁; 田中 伸幸; 野口 弘喜; 上地 優; 井岡 郁夫; 久保 真治; 野村 幹弘*; 八巻 徹也*; 澤田 真一*; et al.

International Journal of Hydrogen Energy, 44(35), p.19141 - 19152, 2019/07

Thermochemical hydrogen production has attracted considerable interest as a clean energy solution to address the challenges of climate change and environmental sustainability. The thermochemical water-splitting iodine-sulfur (IS) process uses heat from nuclear or solar power and thus is a promising next-generation thermochemical hydrogen production method that is independent of fossil fuels and can provide energy security. This paper presents the current state of research and development of the IS process based on membrane techniques using solar energy at a medium temperature of 600$$^{circ}$$C. Membrane design strategies have the most potential for making the IS process using solar energy highly efficient and economical and are illustrated here in detail. Three aspects of membrane design proposed herein for the IS process have led to a considerable improvement of the total thermal efficiency of the process: membrane reactors, membranes, and reaction catalysts. Experimental studies in the applications of these membrane design techniques to the Bunsen reaction, sulfuric acid decomposition, and hydrogen iodide decomposition are discussed.


Visualizing an ignition process of hydrogen jets containing sodium mist by high-speed imaging

土井 大輔; 清野 裕; 宮原 信哉*; 宇埜 正美*

Journal of Nuclear Science and Technology, 56(6), p.521 - 532, 2019/06

In severe accident scenarios for sodium-cooled fast reactors, it is desirable to gradually consume hydrogen generated by various ex-vessel phenomena without posting a challenge to containment integrity. An effective means is combustion of hydrogen jets containing sodium vapor and mist, but previous studies have been limited to determining ignition thresholds experimentally. The aim of this study was to visualize the ignition process in detail to investigate the ignition mechanism of hydrogen-sodium mixed jets. The ignition experiments of the hydrogen jet containing sodium mist were carried out under a condition of little turbulence. The ignition process was measured with an optical measurement system comprised of a high-speed camera and an image intensifier, and a spatial distribution of luminance was analyzed by image processing. Detail observation revealed that sodium mist particles burned as scattering sparks inside the jet and that hydrogen ignited around the mist particles. Additionally, the experimental results and a simple heat balance calculation indicated that the combustion heat of sodium mist particles could ignite the hydrogen as the heterogeneous ignition source in the fuel temperature range where the mist particle formation was promoted.


Interstitial hydrogen atoms in face-centered cubic iron in the Earth's core

生田 大穣*; 大谷 栄治*; 佐野 亜沙美; 柴崎 裕樹*; 寺崎 英紀*; Yuan, L.*; 服部 高典

Scientific Reports (Internet), 9, p.7108_1 - 7108_8, 2019/05

水素は地球の核にある軽元素のひとつである。その重要性にもかかわらず、高圧で鉄格子中の水素を直接観察することはなされていない。われわれは世界で初めて、その場中性子回折法を用いて、12GPaおよび1200Kまでの面心立方(fcc)鉄格子におけるサイト占有率および格子間水素の体積の決定を行った。体心立方晶および二重六方最密相からfcc相への転移温度は、以前に報告されたものよりも高かった。5GPa以下の圧力では、fcc水素化鉄格子(x)中の水素含有量はx$$<$$0.3で小さかったが、圧力の増加と共にx$$>$$0.8まで増加した。水素原子は八面体(O)と四面体(T)の両方のサイトを占める。fcc格子は水素原子1個あたり2.22 $AA $^{3}$$の割合でほぼ直線的に拡大した。これは以前に推定された値(1.9 $AA $^{3}$$/H)よりも大きい。水素溶解による格子膨張は無視できるほど圧力に依存しない。格子間水素による大きな格子膨張は、コアの密度不足を説明する地球のコア内の推定水素含有量を減少させる。改訂された分析は、全コアが海洋質量の80倍の水素を含み、その内訳は外核と内核はそれぞれ79倍と0.8倍である。


Module design of silica membrane reactor for hydrogen production via thermochemical IS process

Odtsetseg, M.; 田中 伸幸; 野村 幹弘*; 久保 真治

International Journal of Hydrogen Energy, 44(21), p.10207 - 10217, 2019/04

The potential of the silica membrane reactors for use in the decomposition of hydrogen iodide (HI) was investigated by simulation with the aim of producing CO$$_{2}$$-free hydrogen via the thermochemical water-splitting iodine-sulfur process. Simulation model validation was done using the data derived from an experimental membrane reactor. The simulated results showed good agreement with the experimental findings. The important process parameters determining the performance of the membrane reactor used for HI decomposition, namely, reaction temperature, total pressures on both the feed side and the permeate side, and HI feed flow rate were investigated theoretically by means of a simulation. It was found that the conversion of HI decomposition can be improved by up to four times (80%) or greater than the equilibrium conversion (20%) at 400$$^{circ}$$C by employing a membrane reactor equipped with a tubular silica membrane. The features to design the membrane reactor module for HI decomposition of thermochemical iodine-sulfur process were discussed under a wide range of operation conditions by evaluating the relationship between HI conversion and number of membrane tubes.


Preliminary combustion analyses using OpenFOAM

Thwe, T. A.; 寺田 敦彦; 日野 竜太郎

JAEA-Technology 2018-012, 45 Pages, 2019/01


原子力発電所に関連するシビアインシデントや製造工程のリスク以外に、原子力廃棄物のリスクも社会を脅かす可能性がある。低レベル及び高レベルの放射性廃棄物を含む核廃棄物の長期保管下では、金属廃棄物の腐食や容器壁自体の腐食及び廃棄物中の水の放射線分解により水素が自発的に発生する。そこで、水素安全及び環境汚染のリスク低減のために、放射性廃棄物容器における水素燃焼爆発の挙動と特性を調べることとした。本報告書では、OpenFOAMを適用し、簡易コンテナー内におけるメタン燃焼の温度, 速度と二酸化炭素分布を調べる数値解析シミュレーションを行った。燃焼シ解析では、LESフレームを備えているFireFoamソルバーを使用した。結果として、容器の高さ及び流入口のサイズが大きくなるとともに平均温度が上昇することが分かった。一方、FireFoamソルバーで行ったメタン、水素及びヘリウムの拡散挙動シミュレーションから、メタンや水素よりもヘリウムのほうが速く拡散することが明らかにした。XiFoamソルバーを利用することにより、化学量論的条件下で立方体燃焼容器における水素空気予混合火炎の火炎伝播半径が得られた。


Quasielastic neutron scattering of brucite to analyse hydrogen transport on the atomic scale

奥地 拓生*; 豊岡 尚敬*; Purevjav, N.*; 柴田 薫

Journal of Applied Crystallography, 51, p.1564 - 1570, 2018/12

 パーセンタイル:100(Chemistry, Multidisciplinary)

中性子準弾性散乱(QENS)は、鉱物結晶格子内で起こる原子スケール水素拡散プロセスを分析するための新規かつ有効な方法であることが実証されている。この方法は、凝縮体中の拡散性が高い水素原子または水分子の拡散頻度および距離を分析するために敏感であると以前から考えられていた。本論文では、水酸基として結晶格子に結合している非常に遅い運動の水素原子の拡散運動を分析する応用研究の結果が示されている。ブルーサイト鉱物( brucite)、Mg(OH)$$_{2}$$では、水素原子の単一の二次元層面内でのジャンプとそれに最も近い次の層へのジャンプの2種類の水素拡散プロセスが観察された。ブルーサイトの結晶構造内で観察されるこれらの拡散プロセスは、層状構造を有する様々な種類の酸化物およびミネラル内で起こる水素拡散現象にQENS測定が適用可能であることを示している。


Computational fluid dynamics analysis for hydrogen deflagration tests at ENACCEF2 facility

Trianti, N.; 佐藤 允俊*; 杉山 智之; 丸山 結

Proceedings of 11th Korea-Japan Symposium on Nuclear Thermal Hydraulics and Safety (NTHAS-11) (Internet), 7 Pages, 2018/11

Simulation techniques have been developed to analyze the deflagration behavior of hydrogen generated during a hypothetical severe accident in nuclear power plants. The CFD analysis was carried out on the hydrogen deflagration experiment performed at the ENACCEF2 facility composed mainly of a vertical cylindrical tube filled with hydrogen-air mixture and nine annular obstacles were placed in the lower part of the tube. The simulation was carried out by the reactingFoam solver of OpenFOAM 3.0, an open source software for the CFD analysis. The RNG (Renormalization group) k-$$varepsilon$$ model was applied for turbulent flow. The interaction of the chemical reaction with the turbulent flow was considered using PaSR (Partial Stirred Reactor) model with 19 elementary reactions for the hydrogen combustion. The analysis result showed the characteristic of flame acceleration by the obstacle region was qualitatively reproduced even though has discrepancy with the experiment.


Stratification break-up by a diffuse buoyant jet; A CFD benchmark exercise

Studer, E.*; 安部 諭; Andreani, M.*; Bharj, J. S.*; Gera, B.*; Ishay, L.*; Kelm, S.*; Kim, J.*; Lu, Y.*; Paliwal, P.*; et al.

Proceedings of 12th International Topical Meeting on Nuclear Reactor Thermal-Hydraulics, Operation and Safety (NUTHOS-12) (USB Flash Drive), 16 Pages, 2018/10

Nuclear engineering research groups were interested in the phenomena of the interaction between a rising jet and a stratified layer located above in order to better understand the underlying mechanisms of hydrogen accumulation and dispersion in a nuclear reactor containment. Previous studies were performed with an upward jet of fluid heavier or lighter than the upper stratified layer. However, in real configurations i.e. the inner part of a nuclear containment, obstacles such as pipes, components as pumps or reservoirs and walls are present, and they can dissipate the initial momentum of the gas release. Consequently, the upward flow pattern can be considered "diffuse" and buoyant, neither pure jet nor pure plume. Therefore, this challenging issue was part of a project called HYMERES, which was launched and conducted in the OECD/NEA framework. Dedicated experiments were performed to study the interaction between a diffuse buoyant jet and two-layer stratification. In the large-scale MISTRA facility, the HM1-1 test series were conducted in which the erosive flow pattern came from a horizontal hot air jet impinging on a vertical cylinder. These experimental results were offered for a blind and open benchmark exercise.


ETSON-MITHYGENE benchmark on simulations of upward flame propagation experiment in the ENACCEF2 experimental facility

Bentaib, A.*; Chaumeix, N.*; Grosseuvres, R.*; Bleyer, A.*; Gastaldo, L.*; Maas, L.*; Jallais, S.*; Vyazmina, E.*; Kudriakov, S.*; Studer, E.*; et al.

Proceedings of 12th International Topical Meeting on Nuclear Reactor Thermal-Hydraulics, Operation and Safety (NUTHOS-12) (USB Flash Drive), 11 Pages, 2018/10

In the framework of the French MITHYGENE project, the new highly instrumented ENACCEF2 facility was built at the Institut de Combustion Aerothermique Reactivite et Environnement (ICARE) of the Centre National de la Recherche Scientifique (CNRS) in Orleans (France) to address the flame propagation in hydrogen combustion during a severe accident. The ENACCEF2 facility is a vertical tube of 7.65 m height and 0.23 m inner diameter. In the lower part of the tube, annular obstacles are installed to promote turbulent flame propagation. At the initiative of the MITHYGENE project consortium and the European Technical Safety Organisation Network (ETSON), a benchmark on hydrogen combustion was organised with the goal to identify the current level of the computational tools in the area of hydrogen combustion simulation under conditions typical for safety considerations for NPP. In the proposed paper, the simulation results obtained by participating organizations, using both Computational Fluid Dynamics (CFD) and lumped-parameter computer codes, are compared to experimental results and analysed.


Experimental validation of the brightness distribution on the surfaces of coupled and decoupled moderators composed of 99.8% parahydrogen at the J-PARC pulsed spallation neutron source

原田 正英; 勅使河原 誠; 大井 元貴; Klinkby, E.*; Zanini, L.*; Batkov, K.*; 及川 健一; 藤 暢輔; 木村 敦; 池田 裕二郎

Nuclear Instruments and Methods in Physics Research A, 903, p.38 - 45, 2018/09

 被引用回数:3 パーセンタイル:7.87(Instruments & Instrumentation)

At the J-PARC pulsed spallation neutron source, liquid hydrogen moderators composed of 99.8% parahydrogen associated with light-water premoderator have been providing high intensity cold and thermal neutron beams. In the design stage, simulations have shown not only high total neutron intensity in the coupled moderator but also a local neutron-brightness increase at the edges. The edge-effect-brightness increase is also exploited in the design of the European Spallation Source (ESS) moderators, which are based on 99.8% parahydrogen, but thin (thickness: 3 cm) to enhance the neutron brightness. In this study, the spatial distribution of the neutron brightness at the surface of the coupled moderator in the J-PARC pulsed spallation neutron source was directly measured with the pinhole geometry to validate the calculated edge-brightness enhancement. The brightness distribution at the moderator surface was clearly observed as predicted by a Monte Carlo simulation, proving the validity of the simulation tools used in the design-optimization process of the J-PARC and ESS moderator.


Influence of Zn injection on PWSCC crack growth rates and oxide film properties of Alloy 600

知見 康弘; 佐藤 賢二*; 笠原 茂樹; 梅原 隆司*; 塙 悟史

Proceedings of Contribution of Materials Investigations and Operating Experience to Light Water NPPs' Safety, Performance and Reliability (FONTEVRAUD-9) (Internet), 10 Pages, 2018/09

一次系冷却水中での応力腐食割れ(PWSCC)進展挙動への亜鉛注入の影響を調べるため、加圧水型軽水炉(PWR)一次系水模擬環境での10%冷間加工600合金の亀裂進展試験を、320$$^{circ}$$C、低濃度(5$$sim$$10ppb)の亜鉛注入、溶存水素濃度(DH)5, 30、及び50cc/kgH$$_{2}$$Oの条件下で実施した。その結果、亀裂進展速度のDH依存性が亜鉛注入なしの試験データに基づく亀裂進展速度の予測値と同様の傾向を示し、実機環境を模擬した低濃度亜鉛注入が亀裂進展挙動に及ぼす影響はほとんど見られなかった。そこで、亀裂進展試験後の試験片の亀裂内及び表面に生成した酸化皮膜の微細組織分析を実施したところ、試験片表面の酸化皮膜からは亜鉛が検出されたが、亀裂内に生成した酸化皮膜からは亜鉛が検出されなかった。このことから、亀裂先端部の酸化皮膜への亜鉛の取り込みがないことが亀裂進展挙動への亜鉛注入の影響が見られない原因であることがわかった。


Recovery of helium refrigerator performance for cryogenic hydrogen system at J-PARC MLF

麻生 智一; 勅使河原 誠; 長谷川 勝一; 武藤 秀生; 青柳 克弘; 野村 一隆; 高田 弘

Journal of Physics; Conference Series, 1021(1), p.012085_1 - 012085_4, 2018/06

At J-PARC's pulsed spallation neutron source, a cryogenic hydrogen system has been operated to provide liquid para-hydrogen (20K and 1.5 MPa) to the moderators since 2008. Typical operating period of the cryogenic hydrogen system was approximately 3 months continuously. However, the pressure differences between No.1, No.2 heat exchangers (HXs) and an adsorber (ADS) in the helium refrigerator had begun to increase rapidly since the beginning of 2015, the refrigerator could not be operated continuously. The impurity in the refrigerator was measured by newly introduced quadrat mass spectrometer, but no significant impurities was observed. We suspected the oil contamination from the helium compressor, as it caused performance degradation of the cryogenic system in other facilities, such as RIKEN, CERN, etc. In the summer outage in 2016, we cleaned the HXs with Freon to remove the oil contamination, and replaced the activate charcoals of ADS and oil separator (OS-5). As a result, the performance of the helium refrigerator was recovered completely.


Stratification breakup by a diffuse buoyant jet; The MISTRA HM1-1 and 1-1bis experiments and their CFD analysis

安部 諭; Studer, E.*; 石垣 将宏; 柴本 泰照; 与能本 泰介

Nuclear Engineering and Design, 331, p.162 - 175, 2018/05

 被引用回数:2 パーセンタイル:16.17(Nuclear Science & Technology)

Density stratification and its breakup are important phenomena to consider in the analysis of the hydrogen distribution during a severe accident. Many previous experimental studies, using helium as mimic gas of hydrogen, focused on the stratification breakup by a vertical or horizontal jet. However, in a real containment vessel, the upward flow pattern can be considered diffuse and buoyant neither pure jet nor pure plume. HM1-1 and HM1-1bis tests in the MISTRA facility were performed to investigate such erosive flow pattern created from a horizontal hot air jet impinging on a vertical cylinder. The experimental results indicated that the jet flow was quickly mixed with the surrounding gas in the lower region of the initial stratification, and deaccelerated by buoyancy force therein. Consequently, the erosive process became slower at the upper region of the initial stratification. Those observed behavior was analyzed using the computational fluid dynamics (CFD) techniques focusing on models for turbulent Schmidt and Prndtl numbers. Some previous studies mentioned that these numbers significantly change in the stratified flow. The changes of $$Sc_{t}$$ and $$Pr_{t}$$ are very important factor to predict the stratification erosion process. The results have indicated that the simulation can be much improved by using appropriate dynamic models for those numbers. This research is a collaboration activity between CEA and JAEA.


The Influence of the air fraction in steam on the growth of the columnar oxide and the adjacent $$alpha$$-Zr(O) layer on Zry-4 fuel cladding at 1273 and 1473 K

Negyesi, M.; 天谷 政樹

Annals of Nuclear Energy, 114, p.52 - 65, 2018/04

 被引用回数:1 パーセンタイル:38.14(Nuclear Science & Technology)

The growth kinetics of the columnar oxide and $$alpha$$-Zr(O) layers of Zry-4 under mixed steam-air conditions at temperatures of 1273 and 1473 K were investigated in this study be means of post-test metallographic measurements. The hydrogen uptake was also determined by the inert gas fusion technique. The kinetics of the columnar oxide layer obeyed a parabolic law for all air fractions at both temperatures. The kinetics of $$alpha$$-Zr(O) layer appeared to deviate slightly from the parabolic law. The parabolic oxidation rate constant of the columnar oxide increased with increasing air fraction, whereas the parabolic oxidation rate constant of $$alpha$$-Zr(O) layer seemed to be independent of the air fraction. Mixed steam-air conditions appeared to enhance hydrogen absorption substantially, especially after the columnar oxide lost its protectiveness.


第4世代原子炉の開発動向,2; 高温ガス炉

國富 一彦; 西原 哲夫; Yan, X.; 橘 幸男; 柴田 大受

日本原子力学会誌, 60(4), p.236 - 240, 2018/04



Conceptual design of the iodine-sulfur process flowsheet with more than 50% thermal efficiency for hydrogen production

笠原 清司; 今井 良行; 鈴木 孝一*; 岩月 仁; 寺田 敦彦; Yan, X.

Nuclear Engineering and Design, 329, p.213 - 222, 2018/04

 パーセンタイル:100(Nuclear Science & Technology)

原子力機構が開発を行っている商用高温ガス炉GTHTR300C(Gas Turbine High Temperature Reactor Cogeneration)を熱源とした、熱化学水素製造IS(iodine-sulfur)プロセスのフロー計算による概念設計を行った。水素製造効率を向上させる以下の革新的技術を提案し、プロセスに組み込んだ:ブンゼン反応排熱の硫酸フラッシュ濃縮への回収、硫酸濃縮塔頂からの硫酸溶液投入による硫酸留出の抑制、ヨウ化水素蒸留塔内でのヨウ素凝縮熱回収。熱物質収支計算により、GTHTR300Cからの170MWの熱によって約31,900Nm$$^{3}$$/hの水素製造が見積もられた。革新的技術と、将来の研究開発により期待される高性能HI濃縮、分解器、熱交換器の採用によって、50.2%の水素製造効率の達成が見込まれた。


Measurements of neutronic characteristics of rectangular and cylindrical coupled hydrogen moderators

甲斐 哲也; 加美山 隆*; 平賀 富士夫*; 大井 元貴; 広田 克也*; 鬼柳 善明*

Journal of Nuclear Science and Technology, 55(3), p.283 - 289, 2018/03

 パーセンタイル:100(Nuclear Science & Technology)

Extensive simulation calculations were performed in the design studies of the coupled hydrogen moderator for the pulsed spallation neutron source of the Japan Proton Accelerator Research Facility (J-PARC). It was indicated that a para-hydrogen moderator had an intensity-enhanced region at the fringe part, and that pulse shapes emitted from a cylindrical para-hydrogen moderator gave higher pulse-peak intensities with narrower pulse widths than those from a rectangular one without penalizing the time-integrated intensities. To validate the peculiar distribution and advantages in pulse shapes experimentally, some measurements were performed at the neutron source of the Hokkaido University electron linear accelerator facility. It was observed that the neutron intensity was enhanced at edges of the para-hydrogen moderators, whereas it decreased at the same part of the ortho-rich-hydrogen moderator, where the dimension of those moderators was 50 mm in thickness and 120 mm in width and height. The spatial distribution and pulse shapes were also measured for a cylindrical coupled para-hydrogen moderator that has the same dimensions as for the coupled moderator employed for J-PARC. The measured results from the cylindrical moderator were consistent with the results obtained in the design studies for the moderator for J-PARC.


Current status of the high intensity pulsed spallation neutron source at J-PARC

高田 弘

Plasma and Fusion Research (Internet), 13(Sp.1), p.2505013_1 - 2505013_8, 2018/03

大強度陽子加速器施設(J-PARC)のパルス核破砕中性子源は、以下に示す独自の特長を有するモデレータを用いて高強度かつ幅の狭いパルス状の冷中性子を供給している。独自の特長とは、(1)100%比率のパラ水素を用いることでピークが高くテイル成分の低い中性子パルスをつくる、(2)直径14cm、高さ12cmの円筒形状とすることで、50.8$$^{circ}$$という広い取り出し角度範囲で高強度の中性子を利用できる、(3)銀-インジウム-カドミウム合金製の中性子吸収材を使用し、幅が狭く、テイル成分の低い中性子パルスをつくる、というものである。実際、低出力運転時の測定によって、1MWの運転時には、結合型モデレータで4.5$$times$$10$$^{12}$$n/cm$$^{2}$$/s/srの中性子束が得られ、ポイズン型モデレータを使用する中性子実験装置(BL08)では$$Delta$$d/d 0.035%の優れた分解能が得られることを確認した。ここで、dは結晶試料内のある方向の格子面と中性子の入射方向とのなす角度に垂直な方向の面間隔を意味する。1MWで年間5000時間の運転を行うという目標の達成に向けて、現在、微少気泡を水銀ターゲットに注入し、ターゲット容器に生じるキャビテーション損傷を抑制する技術開発やターゲット容器構造を溶接部やボルト接続をできるだけ減らす設計改良を行っている。


R&D status in thermochemical water-splitting hydrogen production iodine-sulfur process at JAEA

野口 弘喜; 竹上 弘彰; 笠原 清司; 田中 伸幸; 上地 優; 岩月 仁; 会田 秀樹; 久保 真治

Energy Procedia, 131, p.113 - 118, 2017/12

 被引用回数:3 パーセンタイル:1.43



Hydrogen production tests by hydrogen iodide decomposition membrane reactor equipped with silica-based ceramics membrane

Odtsetseg, M.; 田中 伸幸; 野村 幹弘*; 久保 真治

International Journal of Hydrogen Energy, 42(49), p.29091 - 29100, 2017/12

 被引用回数:2 パーセンタイル:76.91(Chemistry, Physical)


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