論文 - 松根 英樹
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Synthesis and Characterization of Chitosan Cryogels Modified by Tripolyphosphate and Tannic Acid 査読あり 国際共著
Hardi, J., Kiyoyama, S., Matsune, H., & Shiomori, K.
Journal of Chemical Engineering of Japan 57 ( 1 ) 2024年8月
記述言語：英語 掲載種別：研究論文（学術雑誌）
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Takase H., Goya N., Kiyoyama S., Shiomori K., Matsune H.
Gels 10 ( 1 ) 2024年1月
掲載種別：研究論文（学術雑誌） 出版者・発行元：Gels
Hydrophobic cryogels with monolithic supermacropores based on poly-trimethylolpropane trimethacrylate (pTrim) containing 1-(2-Hydroxyl-5-nonyphenyl)ethanone oxime (LIX84-I) were successfully prepared by a cryo-polymerization technique using organic solvents with freezing points between room temperature and around 0 °C as solvents. The prepared cryogels were characterized in terms of macroscopic shape and porous structure. The cryogels had a monolithic supermacroporous structure and high contents of LIX84-I depending on the added amount of the extractant to the monomer solution. The amount of LIX84-I impregnated in the cryogel had a linear relationship with the added amount of LIX84-I in the monomer solution for cryo-polymerization. Cu(II) in the aqueous solution was immediately adsorbed into the cryogel containing LIX84-I.
DOI： 10.3390/gels10010009
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Synthesis of Silver Nanowires using N,N-Dimethylalkylamine 査読あり
Matsune H., Ueno Y., Wakamatsu T., Fujimoto M.A., Shiomori K., Yamamoto T., Kishida M.
Kagaku Kogaku Ronbunshu 50 ( 1 ) 27 - 34 2024年
掲載種別：研究論文（学術雑誌） 出版者・発行元：Kagaku Kogaku Ronbunshu
We report a novel method for the synthesis of silver nanowires (AgNWs). In this method, silver chloride (AgCl) and N,N-dimethyl-dodecylamine hydrochloride (C12H25NMe2·HCl) are used as a silver source and a protecting agent, respectively. Heating of both reagents in N,N-dimethyldodecylamine forms silver chlorocomplex, AgCl1‒nn solving homogeneously in the melting C12H25NMe2·HCl. The addition of the reducing agent, N,N-dibenzylhydroxyamine to the reaction mixture in order to reduce AgCl1‒nn to silver atom (Ag0) gives firstly multiplied twinned nanoparticles (MTPs), and then uniform silver nanowires (AgNWs) with the dimension of 50‒100 nm in thickness and >20 µm in length. Thermogravimetric analysis of the product reveals that highly pure AgNWs containing less organic residues are obtained. We investigate the effects of loading ratios of tertiary amine hydrochlorides to AgCl, the molecular structures of amines, and reaction temperature on the morphologies and yields of the generated AgNWs. We demonstrate that the MTPs are efficiently generated by the reduction reaction of AgCl1‒nn in the presence of tertiary amine hydrochlorides, and that tertiary amine hydrochlorides also play an important role in anisotropic crystal growth of Ag0 to AgNWs through the formation of the MTPs.
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Shiomori K., Matsune H., Inda N.I., Kiyoyama S., Takei T., Yoshida M.
AIP Conference Proceedings 2719 2023年5月
掲載種別：研究論文（学術雑誌） 出版者・発行元：AIP Conference Proceedings
Crosslinked-gel microcapsules immobilized small droplets of phenolic oxime extractant, 1-(2-hydroxy-5-nonylphenyl) ethanone oxime (LIX84-I) were prepared from O/W emulsion using falling-drop method followed by crosslinking of sodium alginate (Na-Alg) by Ca2+ ion and crosslinking of polyvinyl alcohol (PVA) by glutaraldehyde. A lot of fine droplets of LIX84-I were successfully immobilized in the microcapsules. The LIX84-I contents in the microcapsules increased with an increase in the LIX84-I amounts to the aqueous phase. The maximum extracted amounts of Cu(II) increased linearly with the LIX84-I contents with a slope of 1/2 which means two molecules of LIX84-I react with one Cu(II) ion. The extraction rate was not significantly affected by the size of the extractant droplets dispersed in the microcapsules. The microcapsules could be used repeatedly for the extraction and back-extraction of Cu(II).
DOI： 10.1063/5.0133362
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Batchuluun S., Matsune H., Shiomori K., Yasui K., Bayanjargal O.
AIP Conference Proceedings 2719 2023年5月
掲載種別：研究論文（学術雑誌） 出版者・発行元：AIP Conference Proceedings
In order to apply microcapsules as a functional material of cement composites, such as self-healing and heat-transfer-controlling materials, the effect of the addition of microcapsules on the mechanical properties of cement mortar was investigated. Polystyrene microcapsules containing CaCl2 aqueous solution as a microencapsulation substance with monocore and multicore structures were successfully prepared from solid-in-oil-in-water (S/O/W) emulsion by the solvent evaporation method. The compressive strengths of the mortars with and without the microcapsules were measured at various curing times. The compressive strength of the mortar without microcapsules increased with curing time. The compressive strength of the mortar with the microcapsules was lower than that without microcapsules and increased with time. The decrease in the compressive strength increased with the amount of the microcapsules added in the mortar. The self-healing effect of cracked mortar by CaCl2, which would be supplied from the microcapsules due to outer mechanical force making cracks in the mortar and on the microcapsules was not clearly shown in this experiment. However, permeation and leakage of Cl- ion to the surrounding mortar from the microcapsules was observed by mapping analysis of SEM-EDX.
DOI： 10.1063/5.0133363
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Takase H., Watanabe N., Shiomori K., Okamoto Y., Ciptawati E., Matsune H., Umakoshi H.
Colloids and Interfaces 7 ( 1 ) 2023年3月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：Colloids and Interfaces
Here, we prepared hydrophobic cryogel particles with monolithic supermacropores based on poly-trimethylolpropane trimethacrylate (pTrim) by combining the inverse Leidenfrost effect and cryo-polymerization technique. The hydrophobic cryogel particles prepared by adopting this method demonstrated the separation of the stabilized O/W emulsion with surfactant. The prepared cryogel particles were characterized in terms of macroscopic shape and porous structure. It was found that the cryogel particles had a narrow size distribution and a monolithic supermacroporous structure. The hydrophobicity of the cryogel particles was confirmed by placing aqueous and organic droplets on the particles. Where the organic droplet was immediately adsorbed into the particles, the aqueous droplet remained on the surface of the particle due to repelling force. In addition, after it adsorbed the organic droplet the particle was observed, and the organic solvent was diffused into the entire particle. It was indicated that monolithic pores were distributed from the surface to the interior. Regarding the application of the hydrophobic cryogel particles, we demonstrated the separation of a stabilized oil-in-water emulsion, resulting in the successful removal of the organic solvent from the emulsion.
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Matsune H., Yoshida R., Ikemizu R., Shiomori K., Yamamoto T., Kishida M.
Chemistry Letters 52 ( 12 ) 870 - 873 2023年
掲載種別：研究論文（学術雑誌） 出版者・発行元：Chemistry Letters
Colloidal nano-assemblies containing doxorubicin (DOX) are prepared for the first time by co-precipitation with gluconate. The spherical assembly is wrapped with a porous silica layer via sol-gel process, and confined in the formed cage by treatment with copper(II) ions (Cu2+). The reversible linking of DOX with Cu2+ is allowed to suppress the leakage of DOX, but quick release is turned on in response to glutathione (GSH). The synthesized stimulus-responsive nanocapsules are characterized, and examined in a release test with/without GSH and applied to living HeLa cells.
DOI： 10.1246/cl.230322
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Colloidal Trehalose Nanoparticles: Sacrifice Templates for Hollow Silica Nanospheres 査読あり
Yamamoto T., Matsune H., Ikemizu R., Shiomori K., Muraoka E., Kishida M.
Bulletin of the Chemical Society of Japan 96 ( 8 ) 813 - 815 2023年
掲載種別：研究論文（学術雑誌） 出版者・発行元：Bulletin of the Chemical Society of Japan
We demonstrate a trehalose nanoparticle (Tre NP) colloid first prepared by an injection method, and applied to a sacrifice template to create a hollow silica nanosphere. The Tre NP is successfully coated with a uniform layer of silica via sol-gel process, and removed simply by soaking in water, leading to the formation of the hollow nanostructure.
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Takase H., Shiomori K., Okamoto Y., Watanabe N., Matsune H., Umakoshi H.
ACS Applied Polymer Materials 4 ( 10 ) 7081 - 7089 2022年10月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：ACS Applied Polymer Materials
Here, we report a method to prepare cryogel particles with sponge-like mechanical properties, including high porosity and high elasticity. The preparation process of the cryogel particles of poly(2-hydroxythyl methacrylate) can be summarized in the two following steps: preparation of frozen droplets using the inverse Leidenfrost effect, followed by cryo-gelation by frozen polymerization. First, a polymer precursor was dropwise added into bulk liquid nitrogen (-196 °C). Then, frozen droplets were created by the inverse Leidenfrost effect, which were subsequently polymerized in liquid paraffine (-15 °C). After thawing and drying, the cryogel particles were obtained. The monolithic super-macroporous structure was observed by scanning electron microscopy (SEM). The mechanical properties of the cryogel particles were studied via compression-swelling tests. At maximum compression, the particles achieved 94.3% degree of deformation; remarkably, they returned to their original shape under the swelling state. The strategy proposed herein, which combines the inverse Leidenfrost effect with a cryo-polymerization technique, could be applied to prepare various polymer particles without employing surfactants.
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Preferential adsorption of L-tryptophan by L-phospholipid coated porous polymer particles 査読あり
Takase H., Suga K., Matsune H., Umakoshi H., Shiomori K.
Colloids and Surfaces B: Biointerfaces 216 2022年8月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：Colloids and Surfaces B: Biointerfaces
Chiral selective adsorption of L-amino acid, tryptophan (Trp) was achieved using phospholipid membrane-coated porous polymer particles (PPPs). PPPs with numerous pores were prepared by in situ polymerization of divinylbenzene, and then coated with 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC, L-phospholipid) via the impregnation method. Elemental mapping of energy dispersive X-ray (EDX) analysis revealed that DPPC molecules were distributed to the surface and the inner part of PPPs, where almost all the DPPC molecules applied for impregnation were deposited on PPPs. The phospholipid membrane properties of DPPC-PPPs were characterized using the fluorescence probe 6-lauroyl-2-dimethylaminonaphthalene (Laurdan). The results show that DPPC-PPPs possessed a lipid membrane-like environment similar to pure DPPC liposomes, especially at temperatures below 35 °C. DPPC-PPPs slightly adsorbed L-Trp and D-Trp at 45 °C, while DPPC-PPPs significantly adsorbed L-Trp but not D-Trp at 30 °C: enantio excess (e.e.) was 75.0%. The time course of Trp adsorption was investigated: for both enantiomers, similar adsorption behaviors were observed for 30 h, thus suggesting surface adsorption onto DPPC-PPPs. L-Trp adsorption continued after 30 h, suggesting that L-Trp could be distributed in the inner part of DPPC-PPPs. Interestingly, the reused DPPC-PPPs featured improved adsorption performance, suggesting that the deposited DPPC membranes on PPPs could act as chiral selectors for L-Trp. The optical resolution of L-/D-Trp was performed using DPPC-PPPs, resulting in the e.e. of D-Trp was > 60%. Thus, DPPC-PPPs have the potential of chiral selective adsorption of L-amino acid, which can be used as chiral separation materials.
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Takase H., Watanabe N., Shiomori K., Okamoto Y., Matsune H., Umakoshi H.
ACS Omega 8 ( 1 ) 829 - 834 2022年
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：ACS Omega
We have investigated the versatility of a two-step preparation method, without a detergent, that combines both the inverse Leidenfrost effect and the cryogelation technique by using the macroporous particles of different kinds of monomers (four vinyl monomers) or a natural polymer (agarose). First, the precursor of polymers was dropped into liquid nitrogen to prepare the spherical frozen droplet by the inverse Leidenfrost effect. Second, the frozen droplets were cryo-polymerized at the frozen temperature; then, cryogel particles were prepared after thawing. Subsequently, the basic characteristics of the macroporous polymer particles obtained above were compared, focusing on the appearances, porous morphologies, and mechanical properties. It was found that the similar polymer particles could be obtained by the two-step preparation method, while there was a slight difference in their characteristics, depending on the type of monomers. Especially for the mechanical properties, the cryogel particles of the hydrophilic polymer exhibited a shape memory function with sponge-like elasticity, whereas the hydrophobic polymer particles were observed to be cracked after compression (i.e., no shape memory function). This work provides a versatile method of adopting various kinds of monomers and natural polymers for the preparation of macroporous particles. Hence, the method possibly has a potential to prepare and design "tailor-made"macroporous polymer particles for the application purpose.
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Batchuluun S., Yasui K., Matsune H., Shiomori K., Kiyoyama S., Bayanjargal O.
Journal of Chemical Engineering of Japan 55 ( 5 ) 217 - 224 2022年
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：Journal of Chemical Engineering of Japan
Polystyrene microcapsules were prepared by using the solvent evaporation method from S/O/W emulsion which contains fine particles of CaCl2 in the organic phase. The microcapsules were fractionated by their size and permeability of the wall using settling difference in methanol. Further, phase change materials that have two different wet-ability characters were successfully impregnated. The hydrophobic compound was easily impregnated to microcapsules which have hydrophobic wall material. Meanwhile, the hydrophilic compound, which is salt hydrate, was not impregnated to the same microcapsules via direct impregnation but the salt hydrate was successfully impregnated by the volatile exchange impregnation method. Simple thermal properties of the prepared phase change material microcapsules were examined by TGA and DSC methods.
DOI： 10.1252/jcej.21we120
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Enkhzaya S., Matsune H., Shiomori K., Oyuntstseg B.
AIP Conference Proceedings 2360 2021年9月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：AIP Conference Proceedings
This study examined the adsorption of heavy metals and precious metals from aqueous solution by livestock biomass as biosorbents and their treatment effect with reducing chemicals. The adsorption of copper, lead and cadmium was carried out using sheep wool, sheep manure and sheep fat. The copper adsorption was highest among three biosorbents. Sheep wool was treated with an aqueous solution of Na2S, NaOH, NaHSO3, and NaBH4 to enhance the adsorption ability. The Na2S treatment of sheep wool dramatically enhanced the adsorption amount of Au(III) and Cr(III) and was several effective for Cu(II) and Cr(IV). All adsorption results were confirmed with the Langmuir isotherm model in the equilibrium and Pseudo-second order model in the kinetics. From the adsorption properties and ESCA analysis of sheep wool adsorbed each metal, it was confirmed that Au(III) interacted with thiol and amino groups, Cu(II) and Cr(III) with a carboxyl group, and Cr(VI) with the amino group of sheep wool.
DOI： 10.1063/5.0059664
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Batchuluun S., Matsune H., Shiomori K., Bayanjargal O., Baasankhuu T.
Journal of Chemical Engineering of Japan 54 ( 9 ) 517 - 524 2021年9月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：Journal of Chemical Engineering of Japan
Most microcapsule preparation methods produce a population of microcapsules in a bulk solution. To control the microcapsule preparation or obtain an optimal preparation condition, the mechanism of the microcapsule preparation should be investigated. The mechanism is estimated via structure reformation during the preparation process because diameter and wall thickness are drastically altered in the solution. Considering microcapsule applications, some important properties, such as the mechanical properties of microcapsules and release rate of the encapsulated product, depend on the microcapsule structure. In this study, polystyrene microcapsules containing saline water droplets were prepared via the solvent evaporation method from a solid-in-oil-in-water (S/O/W) emulsion system. The microcapsules exhibited a specific structural distribution, which comprised monocore, multicore, and solidcore structures. The structural distribution was altered by the preparation condition. The monocore structure was absolutely dominant owing to the increase in the amount of calcium chloride added in the organic phase. The salt concentration is not the sole controlling factor of the microcapsule structure, as the surfactant and dispersion exerted a significant impact on the microcapsule structure. The structural distribution was automatically analyzed by a machine learning algorithm (MLA). The decision-making time for the microcapsules preparation was shortened by the accelerated structure determination, and the accuracy was improved by increasing the number of counting particles.
DOI： 10.1252/jcej.21we052
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Analysis of the microcapsule structure based on machine learning algorithm 査読あり
Batchuluun S., Matsune H., Shiomori K., Bayanjargal O., Baasankhuu T.
Journal of Physics: Conference Series 1763 ( 1 ) 2021年2月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：Journal of Physics: Conference Series
For the microcapsules preparation process, the mechanism is estimated by structure reformation during the preparation process since diameter and wall thickness drastically changed. Microstructures are recently studied by machine learning techniques. The Hough transformation algorithm is used by other researchers for the preparation of the microcapsules but it is difficult to determine the mechanism by using only a diameter change of the microcapsules. Therefore, one additional way to establish the mechanism is the analysis of the formation of the microcapsule structure. In this study, The Hough transformation algorithm was used for the image segmentation, the simple feature extractions were checked and the support vector machine and the k-nearest neighbors algorithm were used as classifiers in order to analyze the structure of the microcapsules which were prepared by solvent evaporation method from a solid in oil in water, S/O/W, emulsion system. The structural distribution was analyzed by the developed detection method. The microcapsules had a specific structural distribution which are monocore, multicore, and other aggregated structures. The structural distribution was changed by the preparation condition. The monocore structure was dominant by increasing in the amount of water soluble solid particles added in the organic phase.
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Chromium adsorption on sodium sulfide treated sheep wool 査読あり
Enkhzaya S., Matsune H., Shiomori K., Oyuntsetseg B.
Journal of Physics: Conference Series 1763 ( 1 ) 2021年2月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：Journal of Physics: Conference Series
Chromium adsorption from the aqueous phase was evaluated using Mongolian sheep wool as a biosorbent. The wool was chemically treated with sodium sulfide to enhance the adsorption capacity. The surface of the wool was analyzed by SEM. EDX and FTIR were also used for the analysis of differences in the wool after chromium adsorption. Chromium was detected in the wool after adsorption by EDX analysis. FTIR data indicated the intensity change in amide A and amide I, which shows chromium may be adsorbed to the amino and carboxyl groups of the wool. The sodium sulfide treated wool showed better adsorption capacity of chromium(III) than the untreated wool. In the case of chromium(III), the adsorption amount increased with the pH increased, while for chromium(VI), the adsorption value increased with the pH decreased. Kinetic analysis of the adsorption indicated that the removal of chromium followed pseudo-second order kinetic model for the whole contact time range. Langmuir isotherm model was used for the analysis of adsorption equilibrium and the adsorption followed well Langmuir isotherm. This study demonstrates the sodium sulfide treated wool is an effective and low-cost biosorbent for heavy metal adsorption.
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Recent developments of microcapsules and polymer particles for separation medium 査読あり
Shiomori K., Matsune H., Kiyoyama S., Takei T., Yoshida M., Umakoshi H.
Journal of Physics: Conference Series 1763 ( 1 ) 2021年2月
記述言語：日本語 掲載種別：研究論文（学術雑誌） 出版者・発行元：Journal of Physics: Conference Series
Microcapsules and porous polymer particles containing extractants, which are functional molecules to extract target ions or molecules by specific interaction using in solvent extraction process, are expected to be an effective separation medium of various substances from aqueous solution in hydrometallurgical process of harmful or valuable metals and in environmental protection processes from various pollutants. The preparation method, encapsulating materials and application area of these materials has been developed and extended in recent years. Recent topics of this field was been presented. The research on the polymeric particles for separation medium investigated by authors was introduced and showed the structural effect of the polymeric particles containing extractant on the separation performance of metal ion and chiral separation of amino acids by porous particles impregnated with phospholipids.
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Recent developments of microcapsules and polymer particles for separation medium
Shiomori, K., Matsune, H., Kiyoyama, S., Takei, T., Yoshida, M., Umakoshi, H.
Journal of Physics: Conference Series 1763 2021年2月
記述言語：英語 掲載種別：研究論文（学術雑誌）
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Chromium adsorption on sodium sulfide treated sheep wool 査読あり
Enkhzaya S, Matsune H, Shiomori K., Oyuntsetseg B.
Journal of Physics: Conference Series 1763 2021年2月
記述言語：英語 掲載種別：研究論文（学術雑誌）
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Analysis of the microcapsule structure based on machine learning algorithm 査読あり
Batchuluun S., Matsune H., Shiomori K., Bayanjargal O., Baasankhuu T.
Journal of Physics: Conference Series 1763 ( 1,2 ) 2021年2月
記述言語：英語 掲載種別：研究論文（学術雑誌）