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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。


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:0 パーセンタイル:0.02(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.


Development of a membrane reactor with a closed-end silica membrane for nuclear-heated hydrogen production

Myagmarjav, O.; 田中 伸幸; 野村 幹弘*; 野口 弘喜; 今井 良行; 上地 優; 久保 真治; 竹上 弘彰

Progress in Nuclear Energy, 137, p.103772_1 - 103772_7, 2021/07

 被引用回数:1 パーセンタイル:81.22(Nuclear Science & Technology)

Hydrogen production from nuclear energy has attracted considerable interest as a clean energy solution to address the challenges of climate change and environmental sustainability. With respect to the large-scale and economical production of hydrogen using nuclear energy, the thermochemical water-splitting iodine-sulfur (IS) process is a promising method. The IS process uses sulfur and iodine compounds to decompose water into its elemental constituents, hydrogen and oxygen, by using three coupled chemical reactions: the Bunsen reaction; sulfuric acid decomposition; and hydrogen iodide (HI) decomposition. The decomposition of HI is the efficiency-determining step of the process. In this work, a membrane reactor with a silica membrane closed on one end was designed, and its potential for hydrogen production from HI decomposition was explored. In the reactor-module design, only one end of the membrane tube was fixed, while the closed-end of the tube was freely suspended to avoid thermal expansion effects. The closed-end silica membranes were prepared for the first time by a counter-diffusion chemical vapor deposition of hexyltrimethoxysilane. In application, HI conversion of greater than 0.60 was achieved at a decomposition temperature of 400$$^{circ}$$C. Thus, the membrane reactor with closed-end silica membrane was shown to produce a successful equilibrium shift in the production of hydrogen via HI decomposition in the thermochemical IS process.



佐藤 淳也; 塩田 憲司*; 高岡 昌輝*

材料, 70(5), p.406 - 411, 2021/05

アルミノシリケート硬化体は、構造中に有害元素や放射性核種を固定化する特性を有する無機固化材である。本研究では、元素の固定化性能の向上が期待される低Si/Alモル比のアルミノシリケート硬化体を作製するため、化学試薬からSi/Alモル比が0.5の原料を合成することを試みた。作製したSi-Alゲルの化学組成を分析した結果、Si/Alモル比は0.5となり、不純物が少ない非晶質性の材料を合成できた。Si-Alゲルを用いて作製したアルミノシリケート硬化体は5 MPa以上の一軸圧縮強度を示し、Si-Alゲルがアルミノシリケート硬化体の原料として利用可能であることを確認した。Si/Alモル比が1.25のアルミノシリケート硬化体は、緻密な表面構造を有しており、すべての試料中で一軸圧縮強度が最も高くなった。


放射性微粒子の基礎物性解明による廃炉作業リスク低減への貢献(委託研究); 令和元年度英知を結集した原子力科学技術・人材育成推進事業

廃炉環境国際共同研究センター; 茨城大学*

JAEA-Review 2020-033, 84 Pages, 2021/01




Phase-field model for crystallization in alkali disilicate glasses; Li$$_2$$O-2SiO$$_2$$, Na$$_2$$O-2SiO$$_2$$ and K$$_2$$O-2SiO$$_2$$

河口 宗道; 宇埜 正美*

Journal of the Ceramic Society of Japan, 128(10), p.832 - 838, 2020/10

 被引用回数:0 パーセンタイル:0.01(Materials Science, Ceramics)

本研究では、移動度係数($$L$$)を新しく定義することで、溶融酸化物系におけるフェーズフィールド法(PFM)の技術を開発した。一定の移動係数$$L$$を用いたPFM計算から得られた結晶成長速度($$v_0$$)は、normal growthモデルの熱力学的推進力と同程度であった。また$$L$$の温度依存性は、実験から得られた結晶成長速度と$$v_0$$から決定し、その決定した$$L$$を使って、二酸化アルカリケイ酸ガラスのLi$$_2$$O-2SiO$$_2$$, Na$$_2$$O-2SiO$$_2$$, K$$_2$$O-2SiO$$_2$$の結晶成長速度($$v$$)をシミュレーションした。$$v$$の温度依存性は定性的および定量的に非常に良く一致したため、本PFM計算は$$L$$の有効性を実証した。特に、PFM計算によって得られた$$v$$は、融点($$T_{rm m}$$)で増大し、$$T_{rm m}$$-100Kでピークを示した。さらなる温度の下降では、$$v$$は明確に0ms$$^-1$$に近づくことが分かった。この振舞いは、界面のジャンプ過程を表現する$$L$$によって$$v$$が制限されているためである。$$L$$のパラメータ$$B$$の感度についてもPFM計算を行い、$$B$$$$0$$から$$2$$まで増加すると、$$v$$のピークはより急峻に、ピーク温度は高温側にシフトすることが分かった。アルカリ金属の原子番号が増加するにつれてイオンポテンシャルは減少するので、$$L$$のパラメータ$$A$$$$B$$は、それぞれ指数関数的に増加、直線的に減少することになったと考えられる。本計算により$$L$$$$A$$$$B$$は互いに密接な関係であることが分かった。


Adsorption behavior of cesium on hybrid microcapsules in spent fuel solution

大西 貴士; 小山 真一; 三村 均*

日本イオン交換学会誌, 31(3), p.43 - 49, 2020/10

Hybrid microcapsules (H-MCs) are being development for the column separation of Cs from high-level radioactive liquid waste (HLLW). In this paper, adsorption behavior of H-MCs has been evaluated by a batch method in single-element solution and a spent fuel solution prepared from irradiated MOX fuel. Distribution coefficients ($$K_{rm d}$$s) of various metal ion including Cs were determined for three types of H-MCs (AMP-SG (silica gel enclosing ammonium molybdophosphate), AMP-ALG (calcium alginate gel enclosing ammonium molybdophosphate) and AWP-ALG (calcium alginate gel enclosing ammonium tungstophosphate)) in the spent fuel solution. The three types of H-MCs exhibited higher $$K_{rm d}$$s for Cs than those for the other elements in spent fuel solution. The difference of $$K_{rm d}$$ for the specific element (Cs) and the other elements was larger than one order of magnitude. Therefore, chromatographic separation of Cs in the spent fuel solution using a column packed with H-MCs is promising. It was the same tendency between the spent fuel solution and the single-element solution that the $$K_{rm d}$$ value for Cs of AWP-ALG was the largest followed by that of AMP-ALG and that of AMP-SG. Thus, the mechanism of adsorption of Cs onto these H-MCs would not be changed in the presence of FPs and MAs. Therefore, these types of H-MCs can be effective for separation of Cs in the spent fuel solutions.


Investigation of high-temperature chemical interaction of calcium silicate insulation and cesium hydroxide

Rizaal, M.; 中島 邦久; 斉藤 拓巳*; 逢坂 正彦; 岡本 孝司*

Journal of Nuclear Science and Technology, 57(9), p.1062 - 1073, 2020/09

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



Comparison of experimental and simulation results on catalytic HI decomposition in a silica-based ceramic membrane reactor

Myagmarjav, O.; 田中 伸幸; 野村 幹弘*; 久保 真治

International Journal of Hydrogen Energy, 44(59), p.30832 - 30839, 2019/11

 被引用回数:7 パーセンタイル:46.26(Chemistry, Physical)

In this study, the catalytic decomposition of hydrogen iodide was theoretically and experimentally investigated in a silica-based ceramic membrane reactor to assess the reactors suitability for thermochemical hydrogen production. The silica membranes were fabricated by depositing a thin silica layer onto the surface of porous alumina ceramic support tubes via counter-diffusion chemical vapor deposition of hexyltrimethoxysilane. The performance of the silica-based ceramic membrane reactor was evaluated by exploring important operating parameters such as the flow rates of the hydrogen iodide feed and the nitrogen sweep gas. The influence of the flow rates on the hydrogen iodide decomposition conversion was investigated in the lower range of the investigated feed flow rates and in the higher range of the sweep-gas flow rates. The experimental data agreed with the simulation results reasonably well, and both highlighted the possibility of achieving a conversion greater than 0.70 at decomposition temperature of 400$$^{circ}$$C. Therefore, the developed silica-based ceramic membrane reactor could enhance the total thermal efficiency of the thermochemical process.


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:0 パーセンタイル:0(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.


Development of remote sensing technique using radiation resistant optical fibers under high-radiation environment

伊藤 主税; 内藤 裕之; 石川 高史; 伊藤 敬輔; 若井田 育夫

JPS Conference Proceedings (Internet), 24, p.011038_1 - 011038_6, 2019/01



Thermal behavior, structure, dynamic properties of aqueous glycine solutions confined in mesoporous silica MCM-41 investigated by X-ray diffraction and quasi-elastic neutron scattering

吉田 亨次*; 井上 拓也*; 鳥越 基克*; 山田 武*; 柴田 薫; 山口 敏男*

Journal of Chemical Physics, 149(12), p.124502_1 - 124502_10, 2018/09

 被引用回数:2 パーセンタイル:13.74(Chemistry, Physical)

異なる幾つかの、グリシン濃度, pH、および充填率(=グリシン溶液の質量/MCM-41の乾燥質量))をパラメーターとして、メソポーラスシリカ(MCM-41)に閉じ込められたグリシン水溶液の示差走査熱量測定、X線回折および準弾性中性子散乱(QENS)を305-180Kの温度範囲で実施して、グリシン水溶液の熱的挙動, 構造、および動的特性に対する閉じ込め効果を検討した。


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

Myagmarjav, O.; 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:16 パーセンタイル:57.58(Chemistry, Physical)



Preparation of an H$$_{2}$$-permselective silica membrane for the separation of H$$_{2}$$ from the hydrogen iodide decomposition reaction in the iodine-sulfur process

Myagmarjav, O.; 池田 歩*; 田中 伸幸; 久保 真治; 野村 幹弘*

International Journal of Hydrogen Energy, 42(9), p.6012 - 6023, 2017/03

 被引用回数:17 パーセンタイル:59.75(Chemistry, Physical)

A high performance hydrogen-permselective silica membrane derived from hexyltrimethoxysiline (HTMOS) Si-precursor was developed to enhance chemical equilibrium ratio of hydrogen iodide (HI) decomposition in thermochemical water-splitting iodine-sulfur (IS) process. The silica membrane, called the HTMOS membrane, was prepared via a counter diffusion chemical vapor deposition method. The HTMOS membrane prepared at an optimal condition of 450$$^{circ}$$C within 5 min showed highest H$$_{2}$$ permeance of the order of 10$$^{-7}$$ mol Pa$$^{-1}$$ m$$^{-2}$$ s$$^{-1}$$ with a H$$_{2}$$/SF$$_{6}$$ selectivity of 276. It was found that the HTMOS membrane was stable in HI exposure at 400$$^{circ}$$C during 8 h and its HI permeance was the order of 10$$^{-10}$$ mol Pa$$^{-1}$$ m$$^{-2}$$ s$$^{-1}$$. It was demonstrated that the newly developed the HTMOS membrane could be a promising candidate for HI decomposition membrane reactor at working temperature of around 400$$^{circ}$$C.


Post-grouting with colloidal silica at great depth of the Mizunami Underground Research Laboratory, Japan

辻 正邦*; 小林 伸司*; 佐藤 稔紀; 見掛 信一郎; 松井 裕哉

Proceedings of 8th Nordic Grouting Symposium, p.171 - 185, 2016/09



Interaction of Eu(III) ion and non-porous silica; Irreversible sorption of Eu(III) on silica and hydrolysis of silica promoted by Eu(III)

高橋 嘉夫*; 村田 美穂*; 木村 貴海

Journal of Alloys and Compounds, 408-412, p.1246 - 1251, 2006/02

 被引用回数:21 パーセンタイル:75.01(Chemistry, Physical)




長瀬 賢三*; 森田 昇*; 渡部 昭義*; 浅尾 豊信*

JAERI-Tech 2005-052, 99 Pages, 2005/09




Viscosity and density measurements of melts and glasses at high pressure and temperature by using the multi-anvil apparatus and synchrotron X-ray radiation

大谷 栄治*; 鈴木 昭夫*; 安藤 良太*; 浦川 啓*; 舟越 賢一*; 片山 芳則

Advances in High-Pressure Technology for Geophysical Applications, p.195 - 209, 2005/09



Structural studies on liquids and glasses under high pressure and high temperature

片山 芳則; 稲村 泰弘*

Nuclear Instruments and Methods in Physics Research B, 238(1-4), p.154 - 159, 2005/08

 被引用回数:7 パーセンタイル:50.55(Instruments & Instrumentation)



New laser decontamination technique for radioactively contaminated metal surfaces using acid-bearing sodium silicate gel

亀尾 裕; 中島 幹雄; 平林 孝圀*

Journal of Nuclear Science and Technology, 41(9), p.919 - 924, 2004/09

 被引用回数:10 パーセンタイル:58.07(Nuclear Science & Technology)


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