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Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Akutsu, Kazuhiro*; Yamada, Norifumi*; Yamada, Masako*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.
Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05
Supramolecular organization of extractant molecules impacts metal ions separation behavior. Probing bulk and interfacial structures of the relevant systems is expected to provide key insights into the metal ion selectivity and kinetic aspects. The supramolecular features of two solvent extraction systems based on malonamide extractants THMA in toluene and DBMA in n-heptane were studied using small-angle X-ray scattering for the organic bulk phases, as well as interfacial tension and neutron reflectivity measurements for the interfaces. In the bulk solution, THMA forms dimeric/trimeric associates but no aggregates in toluene, while DBMA forms large aggregates in n-heptane. On the other hand, THMA accumulates in a diffuse layer at the interface at high THMA concentration, whereas DBMA forms a compact but thinner layer. After Pd(II) extraction, the thickness of interfacial layers decreases in the case of THMA, and totally vanishes in the case of DBMA. Based on these new structural information, two mechanisms are proposed for Pd(II) and Nd(III) extraction with malonamides. In toluene, THMA associates slightly accumulate in the vicinity of the interface, then coordinate Pd(II) and diffuse into the organic bulk phase. In n-heptane, DBMA aggregates adsorb at the interface then pick up Nd(III) cations in their polar cores and finally diffuse into the bulk.
Kumada, Takayuki; Iwahara, Daisuke*; Nishitsuji, Shotaro*; Akutsu, Kazuhiro*; Miura, Daisuke; Motokawa, Ryuhei; Sugita, Tsuyoshi; Torikai, Naoya*; Amino, Naoya*; Oku, Takayuki; et al.
Journal of Physical Chemistry C, 128(21), p.8797 - 8802, 2024/05
We elucidated the entanglement of polybutadiene and silane coupling agent (SCA) molecules bound to Si substrates using spin-contrast-variation (SCV) neutron reflectivity (NR). In an annealed integral blend film of polybutadiene and SCA, a SCA layer generated on the Si substrate was composed of 70 vol. percent SCA molecules extended perpendicularly from the silicon substrate and entangled with 30 vol. percent polybutadiene molecules. By contrast, in an SCA-precoated polybutadiene film, the SCA-precoated layer is composed of densely packed SCA molecules forming crystal-like structure, and thus did not become entangled with the postcoated polybutadiene molecules. This poor entanglement resulted in poor binding between polybutadiene and Si substrate.
Micheau, C.; Ueda, Yuki; Akutsu, Kazuhiro*; Bourgeois, D.*; Motokawa, Ryuhei
Solvent Extraction and Ion Exchange, 41(2), p.221 - 240, 2023/02
Times Cited Count：1 Percentile：39.98(Chemistry, Multidisciplinary)Kumada, Takayuki; Miura, Daisuke*; Akutsu, Kazuhiro*; Oku, Takayuki; Torikai, Naoya*; Niizeki, Tomotake*
Hamon, 32(4), p.165 - 168, 2022/11
We demonstrated the advantage of spin-contrast-variation neutron reflectometry on the structure analysis of buried interface between resin and porous silica layers. The interface structure was not reproduced by the normal Gaussian model, but by the asymmetric interface model where crosslinked polymer chains neither permeate the pore nor follow the surface roughness of the silica layer.
Kumada, Takayuki; Miura, Daisuke*; Akutsu, Kazuhiro*; Oishi, Kazuki*; Morikawa, Toshiaki*; Kawamura, Yukihiko*; Suzuki, Junichi*; Oku, Takayuki; Torikai, Naoya*; Niizeki, Tomotake*
Journal of Applied Crystallography, 55(5), p.1147 - 1153, 2022/10
Times Cited Count：1 Percentile：26.15(Chemistry, Multidisciplinary)Spin-contrast-variation neutron reflectivity obtains multiple reflectivity curves from a single sample and a single beam source. We used the strong point of the technique to reveal that, although methylated-perhydropolysilazane-derived silica layer has a higher porosity near the interface with acrylic urethane resin, the resin did not permeate the pore network.
Maruyama, Ryuji; Yamazaki, Dai; Aoki, Hiroyuki; Akutsu, Kazuhiro*; Hanashima, Takayasu*; Miyata, Noboru*; Soyama, Kazuhiko; Bigault, T.*; Saerbeck, T.*; Courtois, P.*
Journal of Applied Physics, 130(8), p.083904_1 - 083904_10, 2021/08
Times Cited Count：3 Percentile：25.71(Physics, Applied)Kofu, Maiko; Watanuki, Ryuta*; Sakakibara, Toshiro*; Kawamura, Seiko; Nakajima, Kenji; Matsuura, Masato*; Ueki, Takeshi*; Akutsu, Kazuhiro*; Yamamuro, Osamu*
Scientific Reports (Internet), 11(1), p.12098_1 - 12098_8, 2021/06
Times Cited Count：5 Percentile：53.82(Multidisciplinary Sciences)Maruyama, Ryuji; Yamazaki, Dai; Akutsu, Kazuhiro*; Hanashima, Takayasu*; Miyata, Noboru*; Aoki, Hiroyuki; Soyama, Kazuhiko
JPS Conference Proceedings (Internet), 33, p.011092_1 - 011092_6, 2021/03
no abstracts in English
Kumada, Takayuki; Akutsu, Kazuhiro*; Oishi, Kazuki*; Morikawa, Toshiaki*; Kawamura, Yukihiko*; Sahara, Masae*; Suzuki, Junichi*; Miura, Daisuke*; Torikai, Naoya*
J-PARC 20-02; J-PARC MLF Annual Report 2019, p.38 - 40, 2021/00
Kumada, Takayuki; Miura, Daisuke*; Akutsu, Kazuhiro*; Suzuki, Junichi*; Torikai, Naoya*
Hamon, 30(4), p.207 - 211, 2020/11
We developed a technique of spin-contrast-variation neutron reflectivity (SCV-NR) for structural analyses of multilayer films. The SCV-NR curves of the polystyrene monolayer film were precisely reproduced using a common set of structural parameters and neutron scattering length density at each proton polarization. This result ensures that SCV-NR curves are not deformed by inhomogeneous PH due to the spin-diffusion mechanism. The number of structural parameters of the lamellar microphase-separated poly(styrene-block-isoprene) thin film is too large to determine with a single unpolarized reflectivity curve only. However, these parameters converged through the global analysis of the SCV-NR curves. In this manner, SCV-NR determines the structure of multilayer films while excluding the incorrect structural model that accidentally accounts for a single unpolarized reflectivity curve only.
Akutsu, Kazuhiro*; Kira, Hiroshi*; Miyata, Noboru*; Hanashima, Takayasu*; Miyazaki, Tsukasa*; Kasai, Satoshi*; Yamazaki, Dai; Soyama, Kazuhiko; Aoki, Hiroyuki
Polymers (Internet), 12(10), p.2180_1 - 2180_10, 2020/10
Times Cited Count：2 Percentile：6.56(Polymer Science)Kumada, Takayuki; Akutsu, Kazuhiro*; Oishi, Kazuki*; Morikawa, Toshiaki*; Kawamura, Yukihiko*; Sahara, Masae*; Suzuki, Junichi*; Torikai, Naoya*
Journal of Applied Crystallography, 52(5), p.1054 - 1060, 2019/10
Times Cited Count：3 Percentile：31.93(Chemistry, Multidisciplinary)We developed a technique of spin-contrast-variation neutron reflectometry (SCV-NR). Polarized-neutron reflectivity curves of film samples vary as a function of their proton-polarization P. The P-dependent reflectivity curves of a polystyrene film was precisely reproduced using a common set of structure parameters and the P-dependent neutron scattering length. The reflectivity curve of poly (styrene-block-isoprene) (PSPI) presented a shoulder attributed to holes with the depth corresponding to one period of periodic lamellae on the free surface only at a specific P. In this way, structural information about specific surfaces or interfaces can be obtained by controlling the P.
Akutsu, Kazuhiro*; Cagnes, M.*; Tamura, Kazuhisa; Kanaya, Toshiji*; Darwish, T. A.*
Physical Chemistry Chemical Physics, 21(32), p.17512 - 17516, 2019/08
Times Cited Count：11 Percentile：55.84(Chemistry, Physical)We combined the deuterium labeling and neutron reflectivity techniques to determine the fine structure of the electric double layer structure in an imidazolium ionic liquid (IL). For this, a simple and large scale deuteration method for imidazolium ILs was developed, where the deuteration level can be systematically controlled.
-hetero donor ligand BIZAKobayashi, Toru; Akutsu, Kazuhiro*; Nakase, Masahiko*; Suzuki, Shinichi; Shiwaku, Hideaki; Yaita, Tsuyoshi
Separation Science and Technology, 54(13), p.2077 - 2083, 2019/02
Times Cited Count：5 Percentile：21.84(Chemistry, Multidisciplinary)Development of separation reagent, which can efficiently separate lanthanides, is of increasing importance because it concerns establishment of purification and recycle techniques rare-earth elements. In our research group, several hetero donor type ligands, which have both oxygen and heterocyclic nitrogen atoms as donor atoms, were developed and revealed that this type of ligands show the selective complexation with specific lanthanide. In this paper, we will discuss the lanthaides complexation properties of the hetero donor type ligand containing benzimidazole group as nitrogen donor (
-methyl--phenyl-2-(1
-benzimidazol-2-yl)-pyridine-6-carboxamide) based on structural investigation by crystallography.
Maruyama, Ryuji; Yamazaki, Dai; Akutsu, Kazuhiro*; Hanashima, Takayasu*; Miyata, Noboru*; Aoki, Hiroyuki; Takeda, Masayasu; Soyama, Kazuhiko
Nuclear Instruments and Methods in Physics Research A, 888, p.70 - 78, 2018/04
Times Cited Count：4 Percentile：37.66(Instruments & Instrumentation)The multilayer structure of Fe/Si and Fe/Ge systems fabricated by ion beam sputtering (IBS) was investigated using X-ray and polarized neutron reflectivity measurements and scanning transmission electron microscopy with energy-dispersive X-ray analysis. The obtained result revealed that the incorporation of sputtering gas particles (Ar) in the Ge layer gives rise to a marked reduction in the neutron scattering length density (SLD) and contributes to the SLD contrast between the Fe and Ge layers almost vanishing for spin-down neutrons. This leads to a possibility of fine-tuning of the SLD for the IBS, which is required to realize a high polarization efficiency of a neutron polarizing supermirror. Fe/Ge polarizing supermirror with 
fabricated showed a spin-up reflectivity of 0.70 at the critical momentum transfer. The polarization was higher than 0.985 for the 
range where the correction for the polarization inefficiencies of the beamline works properly.
Akutsu, Kazuhiro*; Adachi, Motoyasu*; Kawakita, Yukinobu
JAEA-Review 2018-002, 36 Pages, 2018/03
JAEA-Review-2018-002.pdf:4.67MB
Since J-PARC started operation for user programs with high-intensity pulsed neutron beams, many material and life science studies have been carried out at J-PARC. Since partial or complete deuteration of organic compounds for contrast variation in the scattering length densities of materials is one of the most effective techniques in the application of neutron scattering analysis, deuterated materials have led to significant progress in our understanding of the structure of novel organic materials. Aiming at accelerating development of deuteration activities in our country, an international workshop "Deuterated Materials Enhancing Neutron Science for Structure Function Applications" was held as a J-PARC Workshop at Ibaraki Quantum Beam Research Center from 19th October to 20th October in 2017. In this workshop, the chemical/biological deuteration activities and recent scientific results of deuterated materials enhancing neutron study in Japan and other countries were discussed by domestic/foreign deuteration and neutron scientists. This is a report of the workshop summarized by organizers.
Mu, J.*; Motokawa, Ryuhei; Akutsu, Kazuhiro*; Nishitsuji, Shotaro*; Masters, A. J.*
Journal of Physical Chemistry B, 122(4), p.1439 - 1452, 2018/02
Times Cited Count：36 Percentile：72.46(Chemistry, Physical)Motokawa, Ryuhei; Kobayashi, Toru; Endo, Hitoshi*; Ikeda, Takashi; Yaita, Tsuyoshi; Suzuki, Shinichi; Narita, Hirokazu*; Akutsu, Kazuhiro*; Heller, W. T.*
Journal of Nuclear Science and Technology, 53(8), p.1205 - 1211, 2016/08
Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)
-butyl phosphate in organic and aqueous environments and its relevance to nuclear extraction processesMu, J.*; Motokawa, Ryuhei; Williams, C. D.*; Akutsu, Kazuhiro*; Nishitsuji, Shotaro*; Masters, A. J.*
Journal of Physical Chemistry B, 120(23), p.5183 - 5193, 2016/06
Times Cited Count：27 Percentile：59.70(Chemistry, Physical)Hattori, Takanori; Akutsu, Kazuhiro*; Suzuki, Junichi*
Bunseki, 2015(2), p.58 - 64, 2015/02
In the J-PARC MLF, 18 beamlines has been constructed and many studies on scientific and industrial use have been performed. This paper introduces the high-pressure science at high-pressure neutron diffractometer "PLANET" and surface/interface structure analysis at vertical sample geometry polarized neutron reflectometer "SHARAKU".
