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Understanding muon diffusion in perovskite oxides below room temperature based on harmonic transition state theory

伊藤 孝; 髭本 亘; 下村 浩一郎*

Physical Review B, 108(22), p.224301_1 - 224301_11, 2023/12

In positive muon spin rotation and relaxation ($$mu^+$$SR) spectroscopy, positive muons ($$mu^+$$) implanted into solid oxides are conventionally treated as immobile spin-probes at interstitial sites below room temperature. This is because each $$mu^+$$ is thought to be tightly bound to an oxygen atom in the host lattice to form a muonic analogue of the hydroxy group. On the basis of this concept, anomalies in $$mu^+$$SR spectra observed in oxides have been attributed in most cases to the intrinsic properties of host materials. On the other hand, global $$mu^+$$ diffusion with an activation energy of $$sim$$0.1~eV has been reported in some chemically-substituted perovskite oxides at cryogenic temperatures, although the reason for the small activation energy despite the formation of the strong O$$mu$$ bond has not yet been quantitatively understood. In this study, we investigated interstitial $$mu^+$$ diffusion in the perovskite oxide lattice using KTaO$$_3$$ cubic perovskite as a model system. We used the $$mu^+$$SR method and density functional theory calculations along with the harmonic transition state theory to study this phenomenon both experimentally and theoretically. Experimental activation energies for global $$mu^+$$ diffusion obtained below room temperature were less than a quarter of the calculated classical potential barrier height for a bottleneck $$mu^+$$ transfer path. The reduction in the effective barrier height could be explained by the harmonic transition state theory with a zero-point energy correction; a significant difference in zero-point energies for $$mu^+$$ at the positions in the O$$mu$$ bonding equilibrium state and a bond-breaking transition state was the primary cause of the reduction. This suggests that the assumption of immobile $$mu^+$$ in solid oxides is not always satisfied since such a significant decrease in diffusion barrier height can also occur in other oxides.


Predictive and inverse modeling of a radionuclide diffusion experiment in crystalline rock at ONKALO (Finland)

Soler, J. M.*; Kek$"a$l$"a$inen, P.*; Pulkkanen, V.-M.*; Moreno, L.*; Iraola, A.*; Trinchero, P.*; Hokr, M.*; $v{R}$$'i$ha, J.*; Havlov$'a$, V.*; Trpko$v{s}$ov$'a$, D.*; et al.

Nuclear Technology, 209(11), p.1765 - 1784, 2023/11

The REPRO-TDE test was performed at a depth of about 400 m in the ONKALO underground research facility in Finland. Synthetic groundwater containing radionuclide tracers (HTO, Cl-36, Na-22, Ba-133, Cs-134) was circulated for about four years in a packed-off interval of the injection borehole. Tracer activities were additionally monitored in two observation boreholes. The test was the subject of a modelling exercise by the SKB GWFTS Task Force. Eleven teams participated in the exercise, using different model concepts and approaches. Predictive model calculations were based on laboratory-based information concerning porosities, diffusion coefficients and sorption partition coefficients. After the experimental results were made available, the teams were able to revise their models to reproduce the observations. General conclusions from these back-analysis calculations include the need for reduced effective diffusion coefficients for Cl-36 compared to those applicable to HTO (anion exclusion), the need to implement weaker sorption for Na-22, compared to results from laboratory batch-sorption experiments, and the observation of large differences between the theoretical initial concentrations for the strongly-sorbing Ba-133 and Cs-134 and the first measured values a few hours after tracer injection. Different teams applied different concepts, concerning mainly the implementation of isotropic vs. anisotropic diffusion, or the possible existence of Borehole Disturbed Zones around the different boreholes. The role of microstructure was also addressed in two of the models.


Cation interdiffusion in uranium-plutonium mixed oxide fuels; Where are we now?

Vauchy, R.; 廣岡 瞬; 松本 卓; 加藤 正人

Frontiers in Nuclear Engineering (Internet), 1, p.1060218_1 - 1060218_18, 2022/12

Diffusion phenomena in uranium-plutonium mixed oxides U$$_{1-y}$$PuyO$$_{2}$$ dictate the physicochemical properties of MOX nuclear fuel throughout manufacturing, irradiation and storage. More precisely, estimating the cation interdiffusion is paramount insofar as it dovetails with the actinide redistribution during sintering and under irradiation. In this paper, we propose a critical review of the existing experimental data of U and Pu interdiffusion coefficients in MOX fuel.


Modelling of the LTDE-SD radionuclide diffusion experiment in crystalline rock at the $"A$sp$"o$ Hard Rock Laboratory (Sweden)

Soler, J. M.*; Meng, S.*; Moreno, L.*; Neretnieks, I.*; Liu, L.*; Kek$"a$l$"a$inen, P.*; Hokr, M.*; $v{R}$$'i$ha, J.*; Vete$v{s}$n$'i$k, A.*; Reimitz, D.*; et al.

Geologica Acta, 20(7), 32 Pages, 2022/07

 被引用回数:2 パーセンタイル:60.41(Geology)

亀裂性岩石中の地下水流動と物質移行のモデル化に関するSKBタスクフォースにおけるTask 9Bは、スウェーデンのエスポ岩盤研究所で実施された原位置長期収着・拡散試験(LTDE-SD)の試験結果のモデル化に焦点をあてたものである。10のモデリングチームによって、異なるモデル概念やコードを用いたモデル化が実施された。モデル化のアプローチは、(1)拡散方程式の解析解、(2)連続多孔質媒体中の数値計算モデル、(3)微細な不均質性(鉱物粒界,微細亀裂の分布等)を考慮した微細構造モデルの大きく3種に分類できる。異なるチームによるモデル化結果から、岩石や亀裂の表面の擾乱影響を含む岩石特性の不均質な分布、微細な亀裂の効果など、様々な異なるモデル概念の比較・評価がなされた。


Predictive modeling of a simple field matrix diffusion experiment addressing radionuclide transport in fractured rock. Is it so straightforward?

Soler, J. M.*; Neretnieks, I.*; Moreno, L.*; Liu, L.*; Meng, S.*; Svensson, U.*; Iraola, A.*; Ebrahimi, K.*; Trinchero, P.*; Molinero, J.*; et al.

Nuclear Technology, 208(6), p.1059 - 1073, 2022/06

 被引用回数:3 パーセンタイル:47.54(Nuclear Science & Technology)



Phase-field mobility for crystal growth rates in undercooled silicates, SiO$$_2$$ and GeO$$_2$$ liquids

河口 宗道; 宇埜 正美*

Journal of Crystal Growth, 585, p.126590_1 - 126590_7, 2022/05

過冷却ケイ酸塩,SiO$$_2$$,GeO$$_2$$融液中の11種類の酸化物または混合酸化物の結晶化におけるフェーズフィールド易動度$$L$$と結晶成長速度をフェーズフィールドモデル(PFM)を用いて計算し、$$L$$の物質依存性を議論した。実験の結晶成長速度と$$L=1$$のPFMシミュレーションから得られた結晶成長速度の比は、両対数プロットで結晶成長における固液界面プロセスの$$frac{TDelta T}{eta}$$のべき乗に比例した。また$$L=A(frac{k_{B}TDelta T}{6pi^{2}lambda^{3}eta T_{m} })^{B}$$のパラメータ$$A$$$$B$$$$A=6.7times 10^{-6}-2.6$$m$$^4$$J$$^{-1}$$s$$^{-1}$$,$$B=0.65-1.3$$であり、材料に固有の値であることが分かった。決定された$$L$$を用いたPFMシミュレーションにより、実験の結晶成長速度を定量的に再現することができた。$$A$$$$T_{m}$$における単位酸素モル質量あたりの陽イオンモル質量の平均の拡散係数と両対数グラフで比例関係にある。$$B$$は化合物中の酸素モル質量あたりの陽イオンのモル質量の総和$$frac{Sigma_{i}M_{i}}{M_{O}}$$に依存する。$$frac{Sigma_{i}M_{i}}{M_{O}}leq 25$$では、陽イオンのモル質量が大きくなるにつれて$$B$$は小さくなる。陽イオンのモル質量は陽イオンの移動の慣性抵抗に比例するため、$$B$$は陽イオンのモル質量の逆数で減少する。$$frac{Sigma_{i}M_{i}}{M_{O}}geq 25$$の重い陽イオンのケイ酸塩の結晶化では、$$B$$は約$$0.67$$で飽和し、$$T_{p}approx 0.9T_{m}$$となる。


Recent studies on fuel properties and irradiation behaviors of Am/Np-bearing MOX

廣岡 瞬; 横山 佳祐; 加藤 正人

Proceedings of International Conference on Fast Reactors and Related Fuel Cycles; Sustainable Clean Energy for the Future (FR22) (Internet), 8 Pages, 2022/04



Tracer diffusion coefficients measurements on LaPO$$_{4}$$-dispersed LATP by means of neutron radiography

Song, F.*; Chen, H.*; 林田 洋寿*; 甲斐 哲也; 篠原 武尚; 薮塚 武史*; 八尾 健*; 高井 茂臣*

Solid State Ionics, 377, p.115873_1 - 115873_6, 2022/04

 被引用回数:0 パーセンタイル:33.33(Chemistry, Physical)

Lithium tracer diffusion coefficients have been measured in Li$$_{1.3}$$Al$$_{0.3}$$Ti$$_{1.7}$$(PO$$_4$$)$$_3$$ (LATP) and LATP - LaPO$$_4$$ composite solid electrolytes in the temperature range between 300$$^{circ}$$C and 500$$^{circ}$$C by means of neutron radiography technique that utilizes the difference in neutron attenuation of $$^6$$Li and $$^7$$Li isotopes. The diffusion coefficient of LATP - LaPO$$_4$$ composite is higher than that of pristine LATP, although the difference is much smaller than that estimated from the room temperature conductivity. This suggests that the bulk diffusion becomes the predominant diffusion mechanism at 300$$^{circ}$$C to 500$$^{circ}$$C instead of the diffusion along the space charge layer formed around the LaPO$$_4$$ dispersants.



門馬 悠一郎*; 坂入 正敏*; 上野 文義; 大谷 恭平

材料と環境, 71(4), p.121 - 125, 2022/04

3Dプリンタを用いて作製した装置で炭素鋼の大気腐食に及ぼす液膜厚さの影響を調査した。新たに作製した装置により、液膜厚さを正確に保持することが可能となった。異なる厚さの液膜で酸素の拡散限界電流密度($$j_{rm lim}$$)とアノード電流密度($$j_{rm anode}$$)を測定した。液膜が薄くなると、$$j_{rm lim}$$は増加し$$j_{rm anode}$$は減少した。$$j_{rm lim}$$と拡散距離の関係から酸素の拡散係数を3.20$$times$$10$$^{-5}$$ cm$$^{2}$$ s$$^{-1}$$と算出した。この結果を用いて、溶存酸素の拡散に影響を与え始める臨界厚さは0.87mmと求められた。


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:2 パーセンタイル:34.75(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.


Experimental analysis on dynamics of liquid molecules adjacent to particles in nanofluids

橋本 俊輔*; 中島 健次; 菊地 龍弥*; 蒲沢 和也*; 柴田 薫; 山田 武*

Journal of Molecular Liquids, 342, p.117580_1 - 117580_8, 2021/11

 被引用回数:3 パーセンタイル:28.4(Chemistry, Physical)



A Scaling approach for retention properties of crystalline rock; Case study of the in-situ long-term sorption and diffusion experiment (LTDE-SD) at the $"A$sp$"o$ Hard Rock Laboratory in Sweden

舘 幸男; 伊藤 剛志*; Gylling, B.*

Water Resources Research, 57(11), p.e2020WR029335_1 - e2020WR029335_20, 2021/11

 被引用回数:2 パーセンタイル:19.4(Environmental Sciences)

本論文では、エスポ岩盤研究所で実施された原位置長期収着・拡散試験(LTDE-SD)のデータセットを用いて、収着及び拡散パラメータを実験室から原位置条件へと条件変換する手法を構築した。亀裂表面と岩石マトリクスの表面近傍の不均質性は、表面近傍での高い間隙率,拡散及び収着特性と、その段階的な変化を仮定した概念モデルによって評価された。非収着性のCl-36と低収着性のNa-22のモデル化結果によって、表面近傍の5mmの擾乱領域における間隙率と拡散係数の変化を考慮した概念モデルの妥当性が確認された。また、これらの陽イオンと陰イオンの拡散係数は、典型的な陽イオン加速と陰イオン排除の傾向を示した。一方で、収着メカニズムの異なる高収着性トレーサー(Cs-137, Ra-226, Ni-63, Np-237)のモデル化結果から、粒径サイズと収着分配係数との相関関係と、その表面近傍の擾乱との関係から条件変換する手法の有効性が確認された。


Dynamics of water in a catalyst layer of a fuel cell by quasielastic neutron scattering

伊藤 華苗; 山田 武*; 篠原 朗大*; 高田 慎一; 川北 至信

Journal of Physical Chemistry C, 125(39), p.21645 - 21652, 2021/10

 被引用回数:2 パーセンタイル:30.86(Chemistry, Physical)

The catalyst layer (CL) in polymer electrolyte fuel cells (PEFCs) plays a critical role in the performance of a PEFC. In this study, we investigate the water dynamics in the CL using quasielastic neutron scattering (QENS) and small-angle neutron scattering. The temperature dependence of the mean square displacement $$<$$u$$^{2}$$$$>$$ shows that the freezing of water does not occur at a melting temperature in the Nafion thin film of the CL, suggesting that the water is confined in a smaller region than $$sim$$15 ${AA}$. The QENS measurements established three kinds of water in the CL: immobile water tightly connected to a sulfonic group, water in a fast mode assigned to free diffusion restricted in a sphere, and water in a slow mode described by a jump diffusion model. Assuming that these three modes were independent, the number of water molecules in each mode was estimated. On discussing the structure and dynamics elucidated in the study, we finally conclude that the coupled model of the fast and slow modes is plausible for describing the diffusion of water confined in the thin Nafion film of the CL.


Evaluation report of Task 9B based on comparisons and analyses of modelling results for the $"A$sp$"o$ HRL LTDE-SD experiments

Soler, J. M.*; Meng, S.*; Moreno, L.*; Neretnieks, I.*; Liu, L.*; Kek$"a$l$"a$inen, P.*; Hokr, M.*; $v{R}$$'i$ha, J.*; Vete$v{s}$n$'i$k, A.*; Reimitz, D.*; et al.

SKB TR-20-17, 71 Pages, 2021/07

亀裂性岩石中の地下水流動と物質移行のモデル化に関するSKBタスクフォースにおけるTask 9Bは、スウェーデンのエスポ岩盤研究所で実施された原位置長期収着・拡散試験(LTDE-SD)の試験結果のモデル化に焦点をあてたものである。10のモデリングチームによって、異なるモデル概念やコードを用いたモデル化が実施された。モデル化のアプローチは、(1)拡散方程式の解析解、(2)連続多孔質媒体中の数値計算モデル、(3)微細な不均質性(鉱物粒界,微細亀裂の分布等)を考慮した微細構造モデルの大きく3種に分類できる。異なるチームによるモデル化結果から、岩石や亀裂の表面の擾乱影響を含む岩石特性の不均質な分布、微細な亀裂の効果など、様々な異なるモデル概念の比較・評価がなされた。



藤本 望*; 福田 航大*; 本多 友貴*; 栃尾 大輔; Ho, H. Q.; 長住 達; 石井 俊晃; 濱本 真平; 中野 優美*; 石塚 悦男

JAEA-Technology 2021-008, 23 Pages, 2021/06





遠藤 貴志*; 舘 幸男; 石寺 孝充; 寺島 元基

日本原子力学会和文論文誌, 20(1), p.9 - 22, 2021/03

デンドリマーを用いた圧縮ベントナイト中のコロイドの拡散・ろ過挙動の評価手法を構築した。サイズが5.7$$sim$$7.2nmのPAMAMデンドリマーコロイドの拡散・ろ過挙動を、塩濃度0.005$$sim$$0.5mol/L NaCl溶液で飽和させた乾燥密度0.8Mg/m$$^{3}$$のベントナイトを対象に、透過拡散試験によって調査した。得られた破過データと内部プロファイルから、デンドリマーコロイドの実効拡散係数とろ過率を導出した。取得された実効拡散係数は、塩濃度とともに増加する傾向を、ろ過率は逆に塩濃度とともに減少する傾向を確認した。これらの傾向は、先行研究で得られたイオンやコロイドの拡散データと整合するほか、塩濃度の変化に伴う間隙構造や静電的相互作用等から推定される傾向と一致するものであり、ここで構築したコロイドの拡散・ろ過挙動の有効性が確認された。


Online measurement of the atmosphere around geopolymers under gamma irradiation

Cantarel, V.; Lambertin, D.*; Labed, V.*; 山岸 功

Journal of Nuclear Science and Technology, 58(1), p.62 - 71, 2021/01

 被引用回数:3 パーセンタイル:36.29(Nuclear Science & Technology)



Extraction mechanism of lanthanide ions into silica-based microparticles studied by single microparticle manipulation and microspectroscopy

大高 稔紀*; 佐藤 辰巳*; 大野 真平; 名越 航平; 安倍 諒治*; 新井 剛*; 渡部 創; 佐野 雄一; 竹内 正行; 中谷 清治*

Analytical Sciences, 35(10), p.1129 - 1133, 2019/10

 被引用回数:7 パーセンタイル:41.13(Chemistry, Analytical)

Single porous silica microparticles coated with styrene-divinylbenzene polymer (SDB) impregnated with octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) were injected into an aqueous 3 mol/L nitric acid solution containing trivalent lanthanide (Ln(III)), as a high-level liquid waste model, using the microcapillary manipulation-injection technique; and the extraction rate of Ln(III), as an Ln(III)-CMPO complex, into the single microparticles was measured by luminescence microspectroscopy. The extraction rate significantly depended on the Ln(III), CMPO, or NO$$_{3}$$$$^{-}$$ concentration, and was analyzed in terms of diffusion in the pores of the microparticles and complex formation of Ln(III). The results indicated that the rate-determining step in Ln(III) extraction was the diffusion in the pore solution of the microparticles.


Optimum temperature for HIP bonding invar alloy and stainless steel

涌井 隆; 石井 秀亮*; 直江 崇; 粉川 広行; 羽賀 勝洋; 若井 栄一; 高田 弘; 二川 正敏

Materials Transactions, 60(6), p.1026 - 1033, 2019/06

 被引用回数:3 パーセンタイル:18.28(Materials Science, Multidisciplinary)

J-PARCの核破砕中性子源で使用する水銀ターゲット容器は、1.3$$times$$1.3$$times$$2.5m$$^{3}$$と大きいため、使用済み容器の廃棄量を低減する観点で、損傷量の大きい前半部を分割できる構造を検討している。分割部のフランジには、高いシール性能(1$$times$$10$$^{-6}$$Pa・m$$^{3}$$/s以下)が必要である。このフランジの材料として、ビーム運転時の熱変形を低減するために低熱膨張材であるインバー合金は有望であるが、弾性係数が低いためボルト締結時の変形が大きくなる。実用上はステンレス鋼で補強するが、HIP接合により広い面積を全面にわたって確実に接合する条件を見出すことが課題であった。そこで、接合温度が異なる試験片(973, 1173, 1373及び1473K)について、引張試験及び数値解析による残留応力評価を行った。973Kで接合した試験片は、拡散層厚さが殆どなく接合界面で破断した。引張強度は、接合温度の上昇とともに減少し、1473Kの場合、約10%低下した。接合面近傍の残留応力は最大50%増加した。これらの結果から、1173Kが最適な接合温度であることを結論付けた。


A Systematic radionuclide migration parameter setting approach for potential siting environments in Japan

浜本 貴史*; 石田 圭輔*; 澁谷 早苗*; 藤崎 淳*; 舘 幸男; 石黒 勝彦*; McKinley, I. G.*

Proceedings of 2019 International High-Level Radioactive Waste Management Conference (IHLRWM 2019) (USB Flash Drive), p.77 - 82, 2019/04

NUMO's recently published safety case involves utilisation of the safety case approach to provide a basis for preparation for future phases of work and development of a template for later, more complete and rigorous, safety cases. Advances include capturing potential siting environments in Site Descriptive Models (SDMs) and focusing post-closure safety assessment methodology on repository designs tailored to these SDMs. Radionuclide-specific parameters in the engineered barrier system (EBS), such as solubilities, sorption and diffusion values, are selected based on established chemical models that take into account evolution of porewater chemistry, alteration of EBS material and different host rock properties. Existing chemical thermodynamic databases developed in Japan have been used for the coupled geochemical and mass transport analyses applied to set these parameters. Nevertheless, in view of fundamental uncertainties in the thermodynamic approach, expert judgment played a key role in the process. This paper discusses the methodology used to set "reasonably conservative" radionuclide migration parameters for the illustrative SDMs, with a focus on chemistry which can be captured in existing models only by introducing significant simplifications.

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