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論文

Impact of interatomic structural characteristics of aluminosilicate hydrate on the mechanical properties of metakaolin-based geopolymer

Kim, G.*; Cho, S.-M.*; Im, S.*; Suh, H.*; 諸岡 聡; 菖蒲 敬久; 兼松 学*; 町田 晃彦*; Bae, S.*

Construction and Building Materials, 411, p.134529_1 - 134529_18, 2024/01

This study explores the influence of the interatomic structure of sodium aluminosilicate hydrate (N-A-S-H) with varying silica contents on the mechanical properties of metakaolin-based geopolymer. Geopolymer pastes comprising Si/Al ratios between 2.0 and 3.0 were synthesized. A larger number of Si-O-Si linkages compared to Si-O-Al linkages and a higher atomic number density were found in the geopolymers with higher silica contents, which enhanced the compressive strength of the geopolymer pastes up to the optimal Si/Al ratio of 2.5. The paste with a Si/Al = 2.5 exhibited a greater portion of Q$$^{4}$$(1Al and 2Al) and denser morphology compared to the other geopolymer pastes. Furthermore, in-situ high-energy synchrotron X-ray scattering experiments were conducted to assess the elastic modulus of the aluminosilicate structure at a local atomic scale. The modulus value in real space decreases with increasing silica contents up to Si/Al = 2.5 and increases with the presence of excessive unreacted silica fume. The modulus value in reciprocal space for the axial and lateral directions both presented a positive value at the geopolymer comprising a Si/Al ratio higher than 2.5, indicating that the load-bearing property of N-A-S-H changed at higher Si/Al ratios. Moreover, the smallest difference between the strains along the axial and lateral directions was detected for the geopolymer with Si/Al = 2.5 in both the real and reciprocal space, owing to the most interconnected and flexible nanostructure, which led to the highest mechanical strength.

論文

Characteristic microstructural phase evolution and the compressive strength development mechanisms of tricalcium silicate pastes under various initial carbonation curing environments

Cho, S.*; Suh, H.*; Im, S.*; Kim, G.*; 兼松 学*; 諸岡 聡; 町田 晃彦*; 菖蒲 敬久; Bae, S.*

Construction and Building Materials, 409, p.133866_1 - 133866_20, 2023/12

The effects of various initial carbonation curing environments on the phase evolution and resulting mechanical characteristics of tricalcium silicate paste were studied. For the analyses of the reaction products and microstructure, synchrotron X-ray diffraction, thermogravimetry, Fourier transform-infrared spectroscopy, scanning electron microscopy with energy dispersive X-ray spectroscopy and high-resolution X-ray computed tomography were utilized. C$$_{3}$$S cured under carbonation environment pressurized by 0.1 MPa showed excellent mechanical properties owing to the highest degree of reaction and homogeneous generation of CaCO$$_{3}$$ with low-Ca/Si calcium silicate hydrates, resulting in a dense matrix with refined pore structure. C$$_{3}$$S paste treated under other carbonation conditions underwent deteriorative microstructural phase transitions, including void evolution by decalcification of C-S-H and an inhomogeneous composition of crystalline phases, resulting in inferior properties.

論文

Insight on the mechanical properties of hierarchical porous calcium-silicate-hydrate pastes according to the Ca/Si molar ratio using ${it in situ}$ synchrotron X-ray scattering and nanoindentation test

Im, S.*; Jee, H.*; Suh, H.*; 兼松 学*; 諸岡 聡; Choe, H.*; 西尾 悠平*; 町田 晃彦*; Kim, J.*; Lim, S.*; et al.

Construction and Building Materials, 365, p.130034_1 - 130034_18, 2023/02

 被引用回数:6 パーセンタイル:65.14(Construction & Building Technology)

Nanocrystalline calcium-silicate-hydrate (C-S-H) is a typical heterogeneous material with a multiscale structure spanning a wide length scale from angstrom to micrometer, and whose structure is determined by the Ca/Si ratio. In this study, we directly applied compressive loads on synthetic C-S-H pastes with Ca/Si ratios of 0.6-1.2 and investigated their mechanical properties using the elastic modulus calculated at three length scale levels (i.e., angstrom to nanometer, micrometer, and millimeter) via in-situ synchrotron X-ray scattering, nanoindentation tests, and strain gauges, respectively. Further, $$^{29}$$Si nuclear magnetic resonance spectroscopy was conducted on the C-S-H pastes to elucidate the alterations in the silicate polymerization. The experimental results confirmed the deformation behavior of the C-S-H paste with different Ca/Si ratios under external loading, which was demonstrated to be transferred from the surface of the pastes to particles owing to the presence of multiscale pores.

論文

Effect of magnesium silicate hydrate (M-S-H) formation on the local atomic arrangements and mechanical properties of calcium silicate hydrate (C-S-H); In situ X-ray scattering study

Kim, G.*; Im, S.*; Jee, H.*; Suh, H.*; Cho, S.*; 兼松 学*; 諸岡 聡; 小山 拓*; 西尾 悠平*; 町田 晃彦*; et al.

Cement and Concrete Research, 159, p.106869_1 - 106869_17, 2022/09

 被引用回数:18 パーセンタイル:91.81(Construction & Building Technology)

This study explored the effect of M-S-H formation on the local atomic arrangements and mechanical properties of C-S-H. The elastic moduli of the samples were calculated using shifted atomic distances (r) and d-spacings (d) acquired by applying an external load on the pastes during X-ray scattering experiments. The experimental results indicated that the crystal structure of C-S-H remained intact with MgCl$$_{2}$$ addition. At the highest Mg/Si ratio (Ca/Si = 0.6, Mg/Si = 0.2), change in the dominant phase occurred from C-S-H to M-S-H because the low pH environment hindered the formation of C-S-H and facilitated the formation of M-S-H. The elastic modulus decreased with increasing Mg/Si ratio up to 0.1 owing to both C-S-H destabilization and low M-S-H content in the samples. Conversely, the elastic modulus increased in the paste synthesized with the highest Mg/Si ratio because considerable M-S-H had formed, which exhibited a higher elastic modulus than C-S-H.

論文

Temperature effects on local structure, phase transformation, and mechanical properties of calcium silicate hydrates

Im, S.*; Jee, H.*; Suh, H.*; 兼松 学*; 諸岡 聡; 小山 拓*; 西尾 悠平*; 町田 晃彦*; Kim, J.*; Bae, S.*

Journal of the American Ceramic Society, 104(9), p.4803 - 4818, 2021/09

 被引用回数:18 パーセンタイル:83.57(Materials Science, Ceramics)

This study aims to elucidate the effect of heating on the local atomic arrangements, structure, phase transformation, and mechanical properties of synthesized calcium-silicate-hydrate (C-S-H). The alteration in the atomic arrangement of the synthesized C-S-H (Ca/Si = 0.8) and the formation of crystalline phases that occurred in three distinct transformation stages of dehydration (105-200 $$^{circ}$$C), decomposition (300-600 $$^{circ}$$C), and recrystallization (700-1000 $$^{circ}$$C) were investigated via powder X-ray diffraction, $$^{29}$$Si nuclear magnetic resonance spectroscopy, and thermogravimetric analysis. Further, the deformation of the local atomic bonding environment and variations in mechanical properties during the three stages were assessed via pair distribution function analysis based on in-situ total X-ray scattering. The results revealed that the C-S-H paste before heating exhibited a lower elastic modulus in real space than that in the reciprocal space in the initial loading stage because water molecules acted as a lubricant in the interlayer. At the dehydration stage, the strain as a function of external loading exhibited irregular deformation owing to the formation of additional pores induced by the evaporation of free moisture. At the decomposition stage, the structural deformation of the main d-spacing (d $$approx$$ 3.0 ${AA}$) was similar to that of the real space before the propagation of microcracks. At the recrystallization stage, the elastic modulus increased to 48 GPa owing to the thermal phase transformation of C-S-H to crystalline $$beta$$-wollastonite. The results provide direct experimental evidence of the micro- and nanostructural deformation behavior of C-S-H pastes after exposure to high temperature under external loading.

論文

Analysis of atomistic structural deformation characteristics of calcium silicate hydrate in 53-year-old tricalcium silicate paste using atomic pair distribution function

Bae, S.*; Jee, H.*; Suh, H.*; 兼松 学*; 城 鮎美*; 町田 晃彦*; 綿貫 徹*; 菖蒲 敬久; 諸岡 聡; Geng, G.*; et al.

Construction and Building Materials, 237, p.117714_1 - 117714_10, 2020/03

 被引用回数:15 パーセンタイル:65.27(Construction & Building Technology)

Although the atomistic structure and the deformation characteristics of calcium silicate hydrates (C-S-H) are of primary interest in cement chemistry, they have not been fully investigated. In this study, pair distribution function (PDF) analysis was conducted on a 53-year-old fully hydrated tricalcium silicate (C$$_{3}$$S) paste using in situ synchrotron high-energy X-ray scattering to probe the atomic structural deformation of C-S-H under external loading. The results were compared with those from our previous PDF study of a 131-day-old C$$_{3}$$S paste in order to elucidate the effect of aging on the mechanical characteristics of C-S-H. Three different strains measured by the strain gauge, by the lattice shifts (d-spacing) in the reciprocal space, and by the shift of the interatomic distance (r) in the real space were compared. In the range of r $$<$$ 20 ${AA}$, where most of the information was derived from C-S-H, the 53-year-old C$$_{3}$$S paste had a higher overall elastic modulus (18.3 GPa) and better resistance to compressive stress than the 131-day-old C$$_{3}$$S paste (elastic modulus: 8.3 GPa). Moreover, it was found that the macroscopic strains of the 53-year-old C$$_{3}$$S paste were presumably induced by mechanical deformation such as microcracks at the macroscale. The results provide experimental evidence for the atomistic and mesoscale mechanical behavior of C-S-H in the early and late ages.

論文

Stacking fault energy analyses of additively manufactured stainless steel 316L and CrCoNi medium entropy alloy using in situ neutron diffraction

Woo, W.*; Jeong, J.-S.*; Kim, D.-K.*; Lee, C. M.*; Choi, S.-H.*; Suh, J.-Y.*; Lee, S. Y.*; Harjo, S.; 川崎 卓郎

Scientific Reports (Internet), 10(1), p.1350_1 - 1350_15, 2020/01

 被引用回数:64 パーセンタイル:94.63(Multidisciplinary Sciences)

Stacking fault energies (SFE) were determined in additively manufactured (AM) stainless steel (SS 316 L) and equiatomic CrCoNi medium-entropy alloys. In situ neutron diffraction was performed to obtain a number of faulting-embedded diffraction peaks simultaneously from a set of (hkl) grains during deformation. The peak profiles diffracted from imperfect crystal structures were analyzed to correlate stacking fault probabilities and mean-square lattice strains to the SFE. The result shows that averaged SFEs are 32.8 mJ/m$$^2$$ for the AM SS 316 L and 15.1 mJ/m$$^2$$ for the AM CrCoNi alloys. Meanwhile, during deformation, the SFE varies from 46 to 21 mJ/m$$^2$$ (AM SS 316 L) and 24 to 11 mJ/m$$^2$$ (AM CrCoNi) from initial to stabilized stages, respectively. The transient SFEs are attributed to the deformation activity changes from dislocation slip to twinning as straining.

論文

Modelling of marine radionuclide dispersion in IAEA MODARIA program; Lessons learnt from the Baltic Sea and Fukushima scenarios

Peri$'a$$~n$ez, R.*; Bezhenar, R.*; Brovchenko, I.*; Duffa, C.*; Iosjpe, M.*; Jung, K. T.*; 小林 卓也; Lamego, F.*; Maderich, V.*; Min, B. I.*; et al.

Science of the Total Environment, 569-570, p.594 - 602, 2016/11

 被引用回数:26 パーセンタイル:63.20(Environmental Sciences)

IAEAのMODARIAプログラムの枠組みの中で、海洋拡散モデルの詳細な相互比較を、チェルノブイリ原子力発電所事故に伴うバルティック海及び東京電力福島第一原子力発電所事故に伴う福島沖海域における放射性物質の海洋汚染について、$$^{137}$$Csを対象として実施した。複数の海洋拡散モデルとしてBOXモデルや3次元力学モデル等の多様なモデルを用いた。バルティック海におけるモデル比較では極めて良好な一致を示したものの、福島沖海域における比較では各研究機関が所有する海況場を入力として計算した結果に大きな相違が確認されたが、海況場を統一することで良好な一致を得た。本研究結果から、複雑な海洋環境において政策決定支援システムとして運用するオペレーショナルモデルの構築には複数のモデルによるシミュレーション結果をアンサンブル平均するマルチモデルアンサンブル手法を採用することが妥当であることが示唆されたが、緊急時対応としてシステムを運用する際には計算負荷の大きいマルチモデルアンサンブル手法は非現実的であり、効果的な予測手法を継続して検討することが課題である。

論文

A New comparison of marine dispersion model performances for Fukushima Dai-ichi releases in the frame of IAEA MODARIA program

Peri$'a$$~n$ez, R.*; Brovchenko, I.*; Duffa, C.*; Jung, K.-T.*; 小林 卓也; Lamego, F.*; Maderich, V.*; Min, B.-I.*; Nies, H.*; Osvath, I.*; et al.

Journal of Environmental Radioactivity, 150, p.247 - 269, 2015/12

 被引用回数:33 パーセンタイル:69.37(Environmental Sciences)

IAEAのMODARIAプログラムの枠組みの中で、海洋拡散モデルの詳細な相互比較を、福島第一原子力発電所事故に伴う放射性物質の海洋放出を適用例として実施した。複数の海洋拡散モデルは、モデル間の相違の原因を評価することで比較した。本目的を達成するために逐次的な拡散実験(段階的に計算条件を複雑化させる)を実行した。また、福島第一原子力発電所事故の海洋汚染を再現する数値実験を、$$^{137}$$Csを対象に実施し、シミュレーション結果の海水と堆積物中の放射性物質濃度を観測値と比較した。その結果、モデル間の相違の主な原因は海流場の計算結果によるものであることが判明した。しかしながら、海流場を統一することでモデル間の相違の最大原因を除去したものの、拡散モデルの数値スキーム(差分法または粒子法)およびそれらの数値解法の相違によるモデル間のわずかな差が残った。

口頭

An Overview of marine modelling activities in IAEA MODARIA Program; Lessons learnt from the Baltic Sea and Fukushima scenarios

Peri$'a$$~n$ez, R.*; Bezhenar, R.*; Brovchenko, I.*; Duffa, C.*; Iosjpe, M.*; Jung, K.-T.*; 小林 卓也; Lamego, F.*; Maderich, V.*; Min, B.-I.*; et al.

no journal, , 

IAEAのMODARIAプログラムの枠組みの中で、海洋拡散モデルの詳細な相互比較を、チェルノブイリ原子力発電所事故に伴うバルティック海及び東京電力福島第一原子力発電所事故に伴う福島沖海域における放射性物質の海洋汚染について、Cs-137を対象として実施した。複数の海洋拡散モデルとしてBOXモデルや3次元力学モデル等の多様なモデルを用いた。バルティック海におけるモデル比較では極めて良好な一致を示したものの、福島沖海域における比較では各研究機関が所有する海況場を入力として計算した結果に大きな相違が確認されたが、海況場を統一することで良好な一致を得た。発表では、緊急時対応としてシステムを運用する際の課題に焦点を当てて報告する。

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