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Ueda, Yuki; Micheau, C.; Akutsu, Kazuhiro*; Tokunaga, Kohei; Yamada, Masako*; Yamada, Norifumi*; Bourgeois, D.*; Motokawa, Ryuhei
Langmuir, 40(46), p.24257 - 24271, 2024/11
Times Cited Count：0 Percentile：0.00(Chemistry, Multidisciplinary)Microscopic structures in liquid-liquid extraction, such as structuration between extractants or extracted complexes in bulk organic phases and at interfaces, can influence macroscopic phenomena, such as the distribution behavior of solutes, including extraction efficiency, selectivity, and phase separation of the organic phase. In this study, we correlated the macroscopic behavior of the extraction of Zr(IV) ions from nitric acid solutions with microscopic structural information in order to understand at the molecular level the key factors contributing to the higher metal ion extraction performance in the fluorous extraction system comprising fluorous phosphate (TFP) in perfluorohexane as compared to the analogous organic extraction system comprising organic phosphate (THP) in n-hexane. Extended X-ray absorption fine structure, neutron reflectometry, and small-angle neutron scattering revealed the local coordination structure around the Zr(IV) ion, the accumulation of extractant molecules at the interface, and the structuration of extractant molecules in the bulk extraction phase, respectively. In the fluorous extraction system, extractant aggregates with were formed after contact with nitric acid. In contrast, in the organic extraction system, only extractant dimers were formed. We speculate that differences in the local coordination structure around the Zr(IV) ion and the structuration of the extractant molecules in the bulk extraction phase contribute to the high Zr(IV) extraction performance in the fluorous extraction system. In particular, the size of the aggregates hardly changed with increasing Zr(IV) concentration in the fluorous phase, which may be closely related to the absence of phase splitting in the fluorous extraction system.
Nankawa, Takuya; Sekine, Yurina; Matsumura, Daiju; Hiroi, Kosuke; Takata, Shinichi; Kamiya, Yoshimi*; Honda, Takayuki*
Langmuir, 40(11), p.5725 - 5730, 2024/03
Times Cited Count：0 Percentile：0.00(Chemistry, Multidisciplinary)The chemical reaction between Fe and lacquer has been used to create the black color lacquer since ancient times. Here, the chemical state of Fe ions in black lacquer was investigated by using X-ray absorption near edge structure (XANES), extended X-ray absorption fine structure (EXAFS), and Fourier transform-infrared (FT-IR) spectroscopy. Fe(II) or Fe(III) was added to the lacquer paste to prepare black lacquer films by air drying, heating, or UV irradiation. The XANES spectral features of all the film samples were similar, meaning that the Fe ions in the samples existed in the trivalent state regardless of the oxidation state of the initially added Fe. The corresponding Fourier transforms of the EXAFS spectra around the Fe K-edge were used to investigate Fe sites in the lacquer films. The spectra of all the film samples were similar shapes, but the peak intensities decreased in the order air dried 
heated UV irradiated films. This result indicates that heating and UV irradiation made the coordination structure of Fe in the lacquer non-uniform, and that heating caused the greatest non-uniformity. The complementary use of XANES, XAFS, and FT-IR spectroscopy is highly effective for non-destructive analysis of black lacquer in precious cultural artifacts.
Goto, Aki*; Michishio, Koji*; Oka, Toshitaka; Tagawa, Masahito*; Yamashita, Shinichi*
Langmuir, 39(34), p.11954 - 11963, 2023/08
Times Cited Count：1 Percentile：17.05(Chemistry, Multidisciplinary)Atomic oxygen (AO) is one of the dominant components of the residual atmosphere in low Earth orbit. AO collides with spacecraft with translational energy of 5 eV, forming nanoscale protrusions on polymeric materials. This study investigated the size of free-volume holes and the layer thickness that interacted with AO for polyethylene (PE), polypropylene (PP), and polystyrene (PS) by positron annihilation lifetime spectroscopy. By the AO irradiation, oxidized layer formed in the surface, and the maximum depth of the oxidized layer for PE and PP were deeper than for PS. The different sizes of free-volume holes would affect the injection depths of AO, resulting in the oxidized layers' thicknesses and surface morphologies.
Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Bauduin, P.*; Girard, L.*; Diat, O.*
Langmuir, 39(31), p.10965 - 10977, 2023/07
Times Cited Count：7 Percentile：74.82(Chemistry, Multidisciplinary)Liu, Y.*; Miyata, Noboru*; Miyazaki, Tsukasa*; Shundo, Atsuomi*; Kawaguchi, Daisuke*; Tanaka, Keiji*; Aoki, Hiroyuki
Langmuir, 39(29), p.10154 - 10162, 2023/06
Times Cited Count：6 Percentile：64.15(Chemistry, Multidisciplinary)Kobayashi, Taishi*; Fushimi, Tomokazu*; Mizukoshi, Hirofumi*; Motokawa, Ryuhei; Sasaki, Takayuki*
Langmuir, 38(48), p.14656 - 14665, 2022/12
Times Cited Count：2 Percentile：17.05(Chemistry, Multidisciplinary)no abstracts in English
Shimokita, Keisuke*; Yamamoto, Katsuhiro*; Miyata, Noboru*; Arima-Osonoi, Hiroshi*; Nakanishi, Yohei*; Takenaka, Mikihito*; Shibata, Motoki*; Yamada, Norifumi*; Seto, Hideki*; Aoki, Hiroyuki; et al.
Langmuir, 38(41), p.12457 - 12465, 2022/10
Times Cited Count：2 Percentile：17.05(Chemistry, Multidisciplinary)Kakiuchi, Takuhiro*; Matoba, Tomoki*; Koyama, Daisuke*; Yamamoto, Yuki*; Yoshigoe, Akitaka
Langmuir, 38(8), p.2642 - 2650, 2022/03
Times Cited Count：2 Percentile：17.05(Chemistry, Multidisciplinary)0xidation processes at the interface and the surface of Si(111) substrate with thin Hf films were studied using photoelectron spectroscopy in conjunction with supersonic oxygen molecular beams (SOMB). The oxidation starts at the outermost Hf layers and produces stoichiometric HfO
. Hf silicates (Hf-O-Si configuration) were generated in the vicinity of the HfO/Si interface in the case of the irradiation of 2.2 eV SOMB. The oxidation of the Si substrate takes place to generate SiO compounds. Si atoms were emitted from the SiO/Si interface region underneath the HfO overlayers to release the stress generated within the strained Si layers. The emitted Si atoms can pass through the HfO overlayers and react with the impinging O gas.
Izumi, Atsushi*; Shudo, Yasuyuki*; Shibayama, Mitsuhiro*; Miyata, Noboru*; Miyazaki, Tsukasa*; Aoki, Hiroyuki
Langmuir, 37(47), p.13867 - 13872, 2021/11
Times Cited Count：3 Percentile：16.65(Chemistry, Multidisciplinary)(001) surface using supersonic seeded oxygen molecular beamKatsube, Daiki*; Ono, Shinya*; Takayanagi, Shuhei*; Ojima, Shoki*; Maeda, Motoyasu*; Origuchi, Naoki*; Ogawa, Arata*; Ikeda, Natsuki*; Aoyagi, Yoshihide*; Kabutoya, Yuito*; et al.
Langmuir, 37(42), p.12313 - 12317, 2021/10
Times Cited Count：3 Percentile：16.65(Chemistry, Multidisciplinary)We investigated the oxidation of oxygen vacancies at the surface of anatase TiO(001) using supersonic seeded molecular beam (SSMB) of oxygen. The oxygen vacancies at the top-surface and sub-surface could be eliminated by the supply of oxygen using an SSMB. These results indicate that the interstitial vacancies can be mostly assigned to oxygen vacancies, which can be effectively eliminated by using an oxygen SSMB. Oxygen vacancies are present on the surface of anatase TiO(001) when it is untreated before transfer to a vacuum chamber. These vacancies, which are stable in the as-grown condition, could also be effectively eliminated using the oxygen SSMB.
Miyazaki, Tsukasa*; Miyata, Noboru*; Arima, Hiroshi*; Kira, Hiroshi*; Ouchi, Keiichi*; Kasai, Satoshi*; Tsumura, Yoshihiro*; Aoki, Hiroyuki
Langmuir, 37(32), p.9873 - 9882, 2021/08
Times Cited Count：7 Percentile：39.87(Chemistry, Multidisciplinary)Aoki, Hiroyuki; Ogawa, Hiroki*; Takenaka, Mikihito*
Langmuir, 37(1), p.196 - 203, 2021/01
Times Cited Count：2 Percentile：10.43(Chemistry, Multidisciplinary)Miyazaki, Tsukasa*; Shimokita, Keisuke*; Yamamoto, Katsuhiro*; Aoki, Hiroyuki; Yamada, Norifumi*; Miyata, Noboru*
Langmuir, 36(49), p.15181 - 15188, 2020/12
Times Cited Count：8 Percentile：34.89(Chemistry, Multidisciplinary)Ito, Kanae; Harada, Masashi*; Yamada, Norifumi*; Kudo, Kenji*; Aoki, Hiroyuki; Kanaya, Toshiji*
Langmuir, 36(43), p.12830 - 12837, 2020/11
Times Cited Count：14 Percentile：54.41(Chemistry, Multidisciplinary)Miyazaki, Tsukasa*; Miyata, Noboru*; Yoshida, Tessei*; Arima, Hiroshi*; Tsumura, Yoshihiro*; Torikai, Naoya*; Aoki, Hiroyuki; Yamamoto, Katsuhiro*; Kanaya, Toshiji*; Kawaguchi, Daisuke*; et al.
Langmuir, 36(13), p.3415 - 3424, 2020/04
Times Cited Count：17 Percentile：61.42(Chemistry, Multidisciplinary)Miyazaki, Tsukasa*; Miyata, Noboru*; Asada, Mitsunori*; Tsumura, Yoshihiro*; Torikai, Naoya*; Aoki, Hiroyuki; Yamamoto, Katsuhiro*; Kanaya, Toshiji*; Kawaguchi, Daisuke*; Tanaka, Keiji*
Langmuir, 35(34), p.11099 - 11107, 2019/08
Times Cited Count：25 Percentile：68.38(Chemistry, Multidisciplinary)Kobayashi, Taishi*; Nakajima, Shogo*; Motokawa, Ryuhei; Matsumura, Daiju; Saito, Takumi*; Sasaki, Takayuki*
Langmuir, 35(24), p.7995 - 8006, 2019/06
Times Cited Count：5 Percentile：19.37(Chemistry, Multidisciplinary)Motokawa, Ryuhei; Endo, Hitoshi*; Yokoyama, Shingo*; Ogawa, Hiroki*; Kobayashi, Toru; Suzuki, Shinichi; Yaita, Tsuyoshi
Langmuir, 30(50), p.15127 - 15134, 2014/12
Times Cited Count：27 Percentile：61.69(Chemistry, Multidisciplinary)Niide, Teppei*; Shimojo, Kojiro; Wakabayashi, Rie*; Goto, Masahiro*; Kamiya, Noriho*
Langmuir, 29(50), p.15596 - 15605, 2013/12
Times Cited Count：13 Percentile：43.08(Chemistry, Multidisciplinary)Maekawa, Yasunari; Suzuki, Yasuyuki; Maeyama, Katsuya*; Yonezawa, Noriyuki*; Yoshida, Masaru
Langmuir, 22(6), p.2832 - 2837, 2006/03
Times Cited Count：6 Percentile：29.80(Chemistry, Multidisciplinary)Chemical modification of the internal surfaces of cylindrical pores with sub-micrometer of pore diameter in PET film was examined. The modification involved the alkylation of the carboxylic acid on the surfaces with the alkylation reagent containing a fluorescent probe, and it was monitored by observing the change in fluorescent emission intensity. When the DMF solution of 4-(bromomethyl)-6,7-dimethoxycoumarin (BrCU), which bore a coumarin fluorophore, was introduced into the pores, the emission and excitation intensities of the membranes increased proportionally with increases of the pore surface areas. Fluorescent spots of about 300 nm in diameter, which were located at the positions of the pores, can be observed in the fluorescence microscope image of the membranes, indicating that highly concentrated fluorescent probes are chemically incorporated on the internal surfaces of the cylindrical pores with 210 nm in diameter in the membranes. In the reactions of the PET surfaces with BrCU, the fluorescent intensities increased with increases of the contact angles. This result indicates that the hydrophilicity of the internal pore surfaces can be qualitatively modified by controlling the change in the fluorescent intensities.
