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Heterogeneous aggregation of humic acids studied by small-angle neutron and X-ray scattering

斉藤 拓巳*; 元川 竜平; 大窪 貴洋*; 三浦 大輔*; 熊田 高之

Environmental Science & Technology, 57(26), p.9802 - 9810, 2023/07

 被引用回数:0 パーセンタイル:0(Engineering, Environmental)

Aggregation of humic acids (HAs) were studied by small-angle neutron and X-ray scattering techniques. The combination of these techniques enables us to examine aggregation structures of heterogeneous HA particles. Two HAs with distinctive compositions were examined; a commercial HA (PAHA) and a HA extracted from deep sedimentary groundwater (HHA). While macroscopic coagulation tests showed that these HAs were stable in solutions except for HHA at pH $$<$$ 6, small-angle neutron scattering (SANS) and X-ray scattering (SAXS) revealed that they formed aggregates with the sizes exceeding sub-micrometer length scale. The SAXS curves of PAHA remarkably varied with pD, whereas the SANS curves did not. With the help of theoretical fittings, it was revealed that PAHA aggregates consisted of two domains: poorly hydrated cores and well-hydrated proton-rich shells. The cores are (dis)aggregated with pD inside the aggregates of the shell. The SANS and SAXS curves of HHA resemble each other, and their intensities at low q increased with a decrease of pD, indicating the formation of homogeneous aggregates. This study revealed that distinctive aggregation behaviors exist in humic substances with heterogeneous structures like PAHA, which is invaluable for their roles in the fate of contaminants or nutrients in aqueous environments.


Microscopic structural changes during the freeze cross-linking reaction in carboxymethyl cellulose nanofiber hydrogels

三浦 大輔*; 関根 由莉奈; 南川 卓也; 杉田 剛; 大場 洋次郎; 廣井 孝介; 大澤 辰彦

Carbohydrate Polymer Technologies and Applications (Internet), 4, p.100251_1 - 100251_9, 2022/12




熊田 高之; 三浦 大輔*; 阿久津 和宏*; 奥 隆之; 鳥飼 直也*; 新関 智丈*

波紋, 32(4), p.165 - 168, 2022/11



Structure analysis of a buried interface between organic and porous inorganic layers using spin-contrast-variation neutron reflectivity

熊田 高之; 三浦 大輔*; 阿久津 和宏*; 大石 一城*; 森川 利明*; 河村 幸彦*; 鈴木 淳市*; 奥 隆之; 鳥飼 直也*; 新関 智丈*

Journal of Applied Crystallography, 55(5), p.1147 - 1153, 2022/10


 被引用回数:1 パーセンタイル:37.59(Chemistry, Multidisciplinary)



Temporal variability of $$^{137}$$Cs concentrations in coastal sediments off Fukushima

鈴木 翔太郎*; 天野 洋典*; 榎本 昌宏*; 松本 陽*; 守岡 良晃*; 佐久間 一幸; 鶴田 忠彦; 帰山 秀樹*; 三浦 輝*; 津旨 大輔*; et al.

Science of the Total Environment, 831, p.154670_1 - 154670_15, 2022/07

 被引用回数:2 パーセンタイル:40.57(Environmental Sciences)

The monthly monitoring data (total 3647 samples) between May. 2011 and Mar. 2020 were analyzed to describe temporal variability of $$^{137}$$Cs concentration in coastal sediments off Fukushima. $$^{137}$$Cs concentration of sediment had decreasing trend, but non-linear model fitting suggested that this decreasing trend showed slower. Additionally, $$^{137}$$Cs concentration were up to 4.08 times greater in shallow sampling sites (7, 10, 20 m depth) following heavy rainfall events (before five months vs. after five months), such as typhoons. These were consistent with increasing particulate $$^{137}$$Cs (P-$$^{137}$$Cs) fluxes from river and increasing dissolved $$^{137}$$Cs (D-$$^{137}$$Cs) concentration in seawater. Finally, the numerical experiment was conducted and revealed that riverine $$^{137}$$Cs input could preserve $$^{137}$$Cs concentration in coastal sediment. These results indicate that riverine $$^{137}$$Cs input via heavy rainfall events is one of the main factors for preserving $$^{137}$$Cs concentration in coastal sediment off Fukushima.


Development of spin-contrast-variation neutron powder diffractometry for extracting the structure factor of hydrogen atoms

三浦 大輔*; 熊田 高之; 関根 由莉奈; 奥 隆之; 高田 慎一; 廣井 孝介; 岩田 高広*

J-PARC 22-02; J-PARC MLF Annual Report 2021, p.6 - 7, 2022/03




三浦 大輔*; 熊田 高之; 岩田 高広*

日本結晶学会誌, 63(4), p.287 - 293, 2021/12



Development of spin-contrast-variation neutron powder diffractometry for extracting the structure factor of hydrogen atoms

三浦 大輔*; 熊田 高之; 関根 由莉奈; 元川 竜平; 中川 洋; 大場 洋次郎; 大原 高志; 高田 慎一; 廣井 孝介; 森川 利明*; et al.

Journal of Applied Crystallography, 54(2), p.454 - 460, 2021/04


 被引用回数:1 パーセンタイル:20.14(Chemistry, Multidisciplinary)



First isolation and analysis of caesium-bearing microparticles from marine samples in the Pacific coastal area near Fukushima Prefecture

三浦 輝*; 石丸 隆*; 伊藤 友加里*; 栗原 雄一; 乙坂 重嘉*; 坂口 綾*; 三角 和弘*; 津旨 大輔*; 久保 篤史*; 桧垣 正吾*; et al.

Scientific Reports (Internet), 11, p.5664_1 - 5664_11, 2021/03

 被引用回数:10 パーセンタイル:69.74(Multidisciplinary Sciences)



Development of spin-contrast-variation neutron reflectometry

熊田 高之; 阿久津 和宏*; 大石 一城*; 森川 利明*; 河村 幸彦*; 佐原 雅恵*; 鈴木 淳市*; 三浦 大輔*; 鳥飼 直也*

J-PARC 20-02; J-PARC MLF Annual Report 2019, p.38 - 40, 2021/00

Neutron reflectivity (NR) is used to determine the nanostructure of surfaces and interfaces of thin film samples. NR has an ad-vantage over X-ray reflectivity for measuring deeply-buried interface of materials. However, it is difficult to determine the structure of complex multiple surface and interfaces of the thin film from a single reflectivity curve. To overcome the problem, we developed a new technique called spin-contrast-variation neutron reflectometry (SCV-NR), which utilizes the property that coherent polarized-neutron scattering length of a proton remarkably varies as a function of the proton polarization, PH, against the neutron polarization direction. As PH increases, the scattering length density (SLD) of each layer proportionally increases with the number density of protons, resulting in the variation of NR curves. The structure of multiple surface and interfaces of a thin film can be determined from the multiple curves.



熊田 高之; 三浦 大輔*; 阿久津 和宏*; 鈴木 淳市*; 鳥飼 直也*

波紋, 30(4), p.207 - 211, 2020/11



Characterization of two types of cesium-bearing microparticles emitted from the Fukushima accident via multiple synchrotron radiation analyses

三浦 輝*; 栗原 雄一; 山本 政儀*; 坂口 綾*; 山口 紀子*; 関澤 央輝*; 新田 清文*; 桧垣 正吾*; 津旨 大輔*; 板井 啓明*; et al.

Scientific Reports (Internet), 10, p.11421_1 - 11421_9, 2020/07

 被引用回数:18 パーセンタイル:72.45(Multidisciplinary Sciences)

A part of radiocesium emitted during the Fukushima nuclear accident was incorporated in glassy microparticles. We tried to understand the radioactive particles systematically by analyzing a large number of particles. Micro-X-ray computed tomography combined with X-ray fluorescence analysis revealed the presence of many voids and iron-rich part within Type-B particles. The $$^{137}$$Cs concentration (Bq mm$$^{-3}$$) of Type-A particles was $$sim$$10,000 times higher than that of Type-B particles. Among the Type-B particles, the spherical ones had higher concentration of volatile elements than the non-spherical ones. These differences suggested that Type-A particles were formed through gas condensation, whereas Type-B particles were formed through melt solidification.


Precise determination of $$^{12}_{Lambda}$$C level structure by $$gamma$$-ray spectroscopy

細見 健二; Ma, Y.*; 味村 周平*; 青木 香苗*; 大樂 誠司*; Fu, Y.*; 藤岡 宏之*; 二ツ川 健太*; 井元 済*; 垣口 豊*; et al.

Progress of Theoretical and Experimental Physics (Internet), 2015(8), p.081D01_1 - 081D01_8, 2015/08

 被引用回数:14 パーセンタイル:67.25(Physics, Multidisciplinary)

$$gamma$$線分光によって$$^{12}_{Lambda}$$Cハイパー核のレベル構造を精密に測定した。ゲルマニウム検出器群Hyperball2を用いて、$$^{12}$$C$$(pi^{+}, K^{+}gamma)$$反応からの4本の$$gamma$$線遷移を同定することに成功した。基底状態スピン二重項$$(2^{-}, 1^{-}_{1})$$のエネルギー間隔は直接遷移$$M1$$$$gamma$$線により、$$161.5pm0.3$$(stat)$$pm0.3$$(syst)keVと測定された。また、励起準位である$$1^{-}_{2}$$$$1^{-}_{3}$$について、それぞれ、$$2832pm3pm4$$, keVと$$6050pm8pm7$$, keVと励起エネルギーを決定した。これらの測定された$$^{12}_{Lambda}$$Cの励起エネルギーは反応分光による$$lambda$$ハイパー核の実験研究において決定的な基準となる。



加藤 聡*; 三浦 大介*; 伊藤 大佐*; 高橋 義明; 和田 幸男

no journal, , 




小林 大輔; 飯田 正義; 高橋 直樹; 吉元 勝起; 根本 良*; 三浦 進*; 沼尾 輝彦*; 中屋敷 浩*

no journal, , 



地下施設建設技術の開発; 幌延深地層研究計画での取組み

稲垣 大介; 津坂 仁和; 三浦 養一*; 名合 牧人*; 進藤 彰久*; 井尻 裕二*; 小池 真史*; 畠中 千野*

no journal, , 



スピンコントラスト変調中性子粉末結晶構造解析; 現状と課題

熊田 高之; 三浦 大輔; 岩田 高広*

no journal, , 



Development of spin-contrast-variation neutron reflectometry for structural analysis of multilayer films

熊田 高之; 阿久津 和宏*; 三浦 大輔*; 鈴木 淳市*; 鳥飼 直也*

no journal, , 

The spin-contrast-variation neutron reflectometry technique was developed for the structural analysis of multilayer films. Polarized-neutron reflectivity curves of film samples vary according to their proton polarization (PH). The PH-dependent reflectivity curves of a polystyrene monolayer film were precisely reproduced using a common set of structural parameters and the PH-dependent neutron scattering length density of polystyrene. Unpolarized reflectivity curves of poly(styrene-block-isoprene) films were reproduced a lot of models. But, the global fit of the PH-dependent multiple reflectivity curves severely restrict the models.



関根 由莉奈; 南川 卓也; 三浦 大輔*; 柚木 俊二*; 杉田 剛; 中川 洋; 山田 鉄兵*

no journal, , 



Gelation mechanism of freeze-crosslinked cellulose nanofiber gels with high compressive strength

三浦 大輔; 南川 卓也; 山田 鉄兵*; 関根 由莉奈

no journal, , 


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