研究者詳細 - 本塚　智

論文 - 本塚　智

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Effective surface functionalization of carbon fibers for fiber/polymer composites with tailor-made interfaces 査読有り

Shiba K., Tagaya M., Samitsu S., Motozuka S.

ChemPlusChem 79 ( 2 ) 197 - 210 2014年02月

記述言語：英語掲載種別：研究論文（学術雑誌）

Composites between carbon fibers (CFs) and heterogeneous materials have been widely studied and their fabrication techniques have been developed. However, their hydrophobic surfaces make it difficult to disperse CFs into hydrophilic resins, which results in weak junctions with ceramics. To develop high-strength composite fibers, it is important to design interfacial chemical bonds. Thus, surface-modification techniques of CFs have recently become the main focus and their interfaces have been characterized by various analytical methods. In this Minireview, various techniques that modify the CF surface by coating with inorganic polymers (metal oxide compounds) are highlighted, and the applications of novel nanocomposite fibers are also described. Furthermore, interfacial bonds between CFs and polymer resins are reviewed and discussed in terms of CF-reinforced plastics and their future prospects. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOI： 10.1002/cplu.201300356

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Effective composite preparation between graphite and iron particles by the interfacial mediation of force-activated oxygen atoms 査読有り

Motozuka S., Tagaya M., Shiba K., Xu Z., Nishikawa M., Yoshioka T., Ikoma T., Tanaka J.

Industrial and Engineering Chemistry Research 53 ( 43 ) 16736 - 16753 2014年01月

記述言語：英語掲載種別：研究論文（学術雑誌）

© 2014 American Chemical Society. Mechanochemically activated graphite (Gp) and iron particle surfaces were prepared, and the Gp/iron composite interfaces were elucidated to utilize new functions. Activated iron particles with the oxygen atoms prepared by a milling under oxygen atmosphere were shown. Alternately, the Gp particles activated by the milling under argon atmosphere easily agglomerated because of the dangling bonds on the edge surfaces. In the composites, the interfacial bonds (e.g., Fe-O-C) between the Gp and iron oxides on the iron were clearly induced while preserving the carbon atom six-ring structures. Furthermore, the molecular orbital calculations suggested that the activated oxygen atoms in the iron oxides effectively abstract hydrogen atoms from the C-H groups of the Gp edge, resulting in the active bare carbon atoms which can form the interfacial bonds; therefore, the interfacial Fe-O-C bonds for a higher adhesive strength were successfully prepared.

DOI： 10.1021/ie501207u

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Effective preparation of graphite nanoparticles using mechanochemical solid-state reactions 査読有り

Motozuka S., Tagaya M., Ogawa N., Fukui K., Nishikawa M., Shiba K., Uehara T., Kobayashi T.

Solid State Communications 190 28 - 32 2014年01月

記述言語：英語掲載種別：研究論文（学術雑誌）

The mechanochemical milling was utilized to control the nanostructures of plate-like graphite (Gp) microparticles in an argon atmosphere and at room temperature. The aggregated Gp nanoparticles were prepared by the simple solid-state process without organic solvent. Electron microscope observations, X-ray diffraction patterns and Raman spectra revealed the fractured plate-like Gp microparticles as well as the Gp microparticles agglomerated to each other through the dissociative edge surfaces by the milling process to finally generate the Gp nanoparticle aggregates. In the process, the ratio of the edge plane surfaces with the dangling bondings to layered internal surfaces clearly increased with the milling. Therefore, the low environmental burden process for preparing the Gp nanoparticle aggregation was achieved. © 2014 Elsevier Ltd.

DOI： 10.1016/j.ssc.2014.03.023

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Efficient methane conversion to hydrogen by the force-activated oxides on iron particle surfaces 査読有り

Motozuka S., Tagaya M., Ikoma T., Morinaga M., Yoshioka T., Tanaka J.

Journal of Physical Chemistry C 117 ( 31 ) 16104 - 16118 2013年08月

記述言語：英語掲載種別：研究論文（学術雑誌）

Mechanochemically activated iron oxide formation on α-iron (Fe) microparticles for the efficient reaction with methane (CH4) was investigated using a simple milling process to successfully clarify the efficient CH4 adsorption as well as the C-H bonding dissociation. First, the oxides with different oxidation degrees (i.e., disordered or ordered iron oxides) were formed on the Fe by mechanochemical milling under an oxygen atmosphere. The surface analyses by X-ray diffraction, Raman, and X-ray photoelectron spectroscopy (XPS) revealed that the surface iron oxides consisted of two phases (α-Fe2O3 and Fe3O 4), and the Fe2O3-like structure was dominantly grown on the near-surface of the disordered iron oxides during the initial oxidation time (0.08 and 0.80 h). Furthermore, the signals from an electron spin resonance analysis suggested dangling bondings on the disordered oxides, indicating the successful formation of the active O sites. Second, the mechanochemical reaction of the resultant iron oxide surfaces with CH 4 was investigated. As a result, the efficient CH4 adsorption as well H2 generation were prominently observed on the disordered oxides, indicating an effectively dissociative adsorption. XPS analysis of the resultant particles revealed that the C-H bonding dissociation dominantly occurred on the near-surface oxygen atoms. Furthermore, using a molecular orbital calculation analysis, the activated O atoms with dangling bondings in the disordered iron oxides were found to affect the C-H dissociation of the adsorbate molecules (e.g., CH4 and CH3•) and exhibit an efficient H2 generation. On the other hand, the O atoms in the ordered lattice could not induce the C-H dissociation of CH3• to produce the equilibrium adsorption/desorption states and lower H2 generation amount, suggesting the importance of both the force-induced activated O atoms and closest interatomic distances. Therefore, we first achieved the efficient mechanochemical decomposition of CH4 and CH3• to generate H2 by the disordered iron oxide surfaces on α-Fe particles. © 2013 American Chemical Society.

DOI： 10.1021/jp405316t

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Surface functionalization of carbon fibers and the composite techniques with polymers 査読有り

Motozuka S., Hashimoto R., Tagaya M., Kobayashi T.

Kobunshi Ronbunshu 70 ( 6 ) 242 - 252 2013年06月

記述言語：英語掲載種別：研究論文（学術雑誌）

composites between carbon fibers (CFs) and heterogeneous materials have been widely researched, and fabrication techniques have been developed. However, because the CF surfaces are hydrophobic, they poorly disperse into hydrophilic resins and do not form junctions with ceramics. For designing and developing high-strength composites, it is important to investigate and design the interfacial chemical bonds. Thus, recently, research focusses on surface modification and coating techniques of CFs. In this review paper, various surface modification and coating by inorganic polymers (metal oxide compounds) were highlighted to focus the functionalization of the CF surfaces. The applications for novel composite materials was also investigated. Furthermore, the interfacial bonding techniques between CF and polymer resin for carbon fiber reinforced plastic and their future perspectives are reviewed and discussed. ©2013, The Society of Polymer Science, Japan.

DOI： 10.1295/koron.70.242

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Effective functionalization of disordered oxide lattices on iron particle surfaces using mechanochemical reactions 査読有り

Motozuka S., Tagaya M., Nishiyama H., Nishikawa M., Ikoma T., Yoshioka T., Samitsu S., Tanaka J.

Journal of Physical Chemistry C 117 ( 19 ) 9908 - 9919 2013年05月

記述言語：英語掲載種別：研究論文（学術雑誌）

The mechanochemical surface functionalization of iron oxides with disordered lattices on bare iron (Fe) particles was investigated using simple milling processes to clarify the formation mechanism of the oxide layer and investigate the near-surface models with different states. The homogeneous α-Fe particles at the milling equilibrium were first prepared under an argon atmosphere. After the subsequent milling reaction of the particles with oxygen molecules, the surface analyses by X-ray diffraction and Raman and X-ray photoelectron spectroscopies revealed that the near-surface layers consisted of two iron oxide phases (α-Fe2O3 and Fe 3O4) through oxygen atom diffusion, and the α-Fe2O3 was dominantly grown on the near surface. During the initial reaction, the signals from an electron spin resonance suggested the dangling bond formation on α-Fe2O3. The oxygen atoms effectively induce disordered lattices in the local area to form oxidized Fe3+ clusters, and the geometric distortion formed the dangling bonds, which were theoretically supported by a molecular orbital calculation to elucidate the increase in the unpaired electron sites on the α-Fe2O3. Therefore, the defective Fe3+ ions induced by the lattice mismatching between the clusters and bare α-Fe are found to form the disordered lattice that contains the oxygen atoms with unpaired electrons, which are successfully induced by the near-surface strain based on the simple mechanochemical reactions. The patterns of surface activation of the Fe particle surfaces by oxidization will be capable of novel chemical reactions by selective oxygen insertion as well as deep oxidation. © 2013 American Chemical Society.

DOI： 10.1021/jp401655m

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Mechanochemical fabrication of iron-graphite composites 査読有り

Motozuka S., Tagaya M., Ikoma T., Yoshioka T., Xu Z., Morinaga M., Tanaka J.

Journal of Composite Materials 47 ( 10 ) 1241 - 1246 2013年05月

記述言語：英語掲載種別：研究論文（学術雑誌）

The fabrication of iron-graphite composites was investigated using a milling process. Based on the milling time of the process, the average particle size of the host iron particles decreased to 10 μm. The size of the graphite particles decreased to a nanometer scale, resulting in the graphite strongly adhering to the iron surfaces. Raman spectra revealed that the graphite aromatic ring structure disappeared and the iron near-surface layer was changed to iron oxide phases. The dangling bond of the fragmented graphite combined with the oxidized iron surface by interfacial binding to efficiently form the interfacial composites. © The Author(s) 2012 Reprints and permissions: sagepub.co.uk/journalsPermissions.nav.

DOI： 10.1177/0021998312446502

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Mechanochemical fabrication of carbon fiber/nylon-6 composites with interfacial bondings 査読有り

Motozuka S., Tagaya M., Hotta Y., Morinaga M., Ikoma T., Honma T., Daimon T., Tanaka J.

Industrial and Engineering Chemistry Research 52 ( 5 ) 2182 - 2189 2013年02月

記述言語：英語掲載種別：研究論文（学術雑誌）

The mechanochemical fabrication of the composites between carbon fibers (CFs) and nylon-6 (N6) was investigated using a milling process. By the milling, defected surfaces were generated on CFs to obtain the homogeneous length with preserving the cylindrical shape of CF. Fourier transform infrared spectra revealed that the band intensities due to C-O, C-N and O-H bondings increased with the milling. The band position of C-N was shifted to a higher wavenumber, while that of C-O did not change, implying that the main chain of N6 was dissociated at the C-N neighboring the C-O bonds by the force, and subsequently, new bonds between the N atoms of the activated N6 and the C atoms on CFs would be formed. Therefore, the efficient fabrication of the CF/N6 composite fibers with the interfacial bondings was achieved using the mechanochemical reaction. © 2013 American Chemical Society.

DOI： 10.1021/ie301333n

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Methane adsorption and dissociation on mechanochemically activated iron-particle surfaces 査読有り

Motozuka S., Tagaya M., Morinaga M., Lkoma T., Yoshioka T., Tanaka J.

International Journal of Powder Metallurgy 48 ( 6 ) 21 - 29 2012年11月

記述言語：英語掲載種別：研究論文（学術雑誌）

Experimental and theoretical studies of the interfacial reactions between methane and mechanochemically activated iron particles were investigated using a milling technique and a discrete variational molecular orbital calculation. The particles were milled in a stainless steel vessel under a methane atmosphere. Scanning electron microscope (SEM) images revealed that the particles welded together to form larger particles and subsequently fractured into smaller homogeneous particles. The inner pressure of the vessel decreased with increasing milling time, indicative of methane adsorption on the particle surfaces and hydrogen was detected by gas chromatog-raphy. Two possible reactions promoted by milling are postulates: (i) fixation of adsorptive methane on the iron particles, and (iij methane conversion to hydrogen on the naturally oxidized iron. A bond overlap population (BOP) calculation was performed to evaluate the molecular orbital interactions between the methane and iron-particle surfaces. The covalent BOP exhibited a maximum positive value at a distance of 0.15 nm between the hydrogen atom of tetrahedral vertex and the iron atom facing each other at their interface, indicating methane adsorption on the iron particle surfaces. The BOP values between the hydrogen atoms of tetrahedral plane (not facing the iron) and carbon atom of methane decreased slightly with decreasing distance, indicating a dissociative adsorption state and weakened strength of the covalent C-H bond. These phenomena would be affected primarily by the strain in the iron particles and the forces between the methane and the near-surface iron and oxygen atoms. Therefore, methane adsorption and dissociation at the interface are consistent with the mechanochemical conversion of methane to hydrogen on the mechanochemically activated iron-particle surfaces.

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Preparation of copper-graphite composite particles by milling process 査読有り

Motozuka S., Tagaya M., Ikoma T., Yoshioka T., Xu Z., Tanaka J.

Journal of Composite Materials 46 ( 22 ) 2829 - 2834 2012年10月

記述言語：英語掲載種別：研究論文（学術雑誌）

The fabrication of copper-graphite composites by a milling process was investigated using a centrifugal ball mill. The copper particles were homogeneously milled in a graphite vessel, and the reaction time was varied. Scanning electron microscopy images clearly revealed that a fragment of graphite ground by the copper particle adheres to the copper particle surface, indicating the formation of a copper-graphite composite. The composite graphite amount per 1 g of copper particles increased to 0.46 mg at the milling time 5 min, and subsequently decreased to 0.25 mg at 60 min, indicating the suitable milling-time for the interfacial adhesion. When using only the copper particles, the naturally oxidized layer on the surface decreased with milling. On the other hand, when using only the graphite, the characteristic graphite structure is disrupted and the defect structure increased with milling. Thus, the new copper surface generated by milling strongly reacts with the defect structure of the graphite. It is suggested that the interfacial bonding between the copper and graphite was attributed to a Van der Waals attraction and/or binding force due to oxygen atoms located at the interface. © The Author(s) 2012 Reprints and permissions: sagepub.co.uk/journalsPermissions.nav.

DOI： 10.1177/0021998311432947

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Efficient incorporation of monomeric anthracene into nanoporous silica/surfactant nanocomposite spheres using a mechanochemical solid state reaction 査読有り

Tagaya M., Motozuka S., Kobayashi T., Ikoma T., Tanaka J.

Journal of Materials Chemistry 22 ( 36 ) 18741 - 18743 2012年09月

記述言語：英語掲載種別：研究論文（学術雑誌）

The incorporation of anthracene (Ant) into nanoporous silica/surfactant nanocomposite spheres was successfully achieved using a mechanochemical solid state reaction. The Ant molecules were incorporated into the nanopores while preserving the silica nanostructures, indicating the effective hydrophobic interactions with the alkyl chains of the surfactant. The blue photoluminescence intensity due to the monomer state was enhanced by increasing the mechanochemical milling force, suggesting this is an efficient preparation method for a luminescent medium by monomeric assembly of the Ant molecules. © The Royal Society of Chemistry.

DOI： 10.1039/c2jm34155g

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Mechanochemical preparation of 8-hydroxyquinoline/hydroxyapatite hybrid nanocrystals and their photofunctional interfaces 査読有り

Tagaya M., Motozuka S., Kobayashi T., Ikoma T., Tanaka J.

Industrial and Engineering Chemistry Research 51 ( 34 ) 11294 - 11300 2012年08月

記述言語：英語掲載種別：研究論文（学術雑誌）

Hybrid nanocrystals of 8-hydroxyquinoline (8Hq) molecules and hydroxyapatite nanocrystals (HAp) were successfully prepared by a mechanochemical solid-state reaction. The hybrid nanocrystals exhibit a significant thermal stability and efficient photoluminescence peak at 500 nm, which were attributed to metal-ligand charge transfer at the interface between the oxygen atoms of 8Hq and the calcium ions of HAp, and the interfacial photofunctions were mechanochemically controlled. The interfacial bonding structures were also supported by a DV-Xα molecular orbital calculation. © 2012 American Chemical Society.

DOI： 10.1021/ie301755z

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Effect of glutaraldehyde on properties of membranes prepared from fish scale collagen 査読有り

Xu Z., Ikoma T., Yoshioka T., Tagaya M., Motozuka S., Matsumoto R., Uemura T., Tanaka J.

Materials Research Society Symposium Proceedings 1418 189 - 194 2012年08月

記述言語：英語掲載種別：研究論文（国際会議プロシーディングス）

Collagen fibril membranes (CFMs) with a high mechanical property were fabricated with a lateral face evaporation method, in which type I atelocollagen extracted from tilapia scales was used. The density and thickness of the CFM obtained were 0.51 ± 0.04 mg/cm 3 and 50 ± 5 μm. The collagen fibrils in the CFM had a similar periodic stripped pattern of 67 nm with native collagen fibrils. The CFM was crosslinked in gaseous glutaraldehyde for different duration in order to increase the mechanical property. The crosslinking degrees of the CFMs analyzed by free amino groups gradually increased to 70.3 % against the exposure duration until 6 hours, and reached a plateau. The denaturation temperatures of the CFMs with the crosslinking degrees at 20.4 % to 43% were linearly increased from 49°C to 75°C. The tensile strength of the CFMs was slightly improved until the crosslinking degree at 33.3 % and then the tensile strength rapidly increased to be 68 MPa. It was suggested that a percolation phenomenon took place in the CFMs by crosslinking of collagen fibrils with polymerized GA molecules. © 2012 Materials Research Society.

DOI： 10.1557/opl.2012.396

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Synthesis and luminescence properties of Eu(III)-doped nanoporous silica spheres 査読有り

Tagaya M., Ikoma T., Yoshioka T., Motozuka S., Xu Z., Minami F., Tanaka J.

Journal of Colloid and Interface Science 363 ( 2 ) 456 - 464 2011年11月

記述言語：英語掲載種別：研究論文（学術雑誌）

Europium (III) (Eu 3+)-doped nanoporous silica spheres were synthesized, and the states of Eu 3+ ions in the silica framework structure were investigated. The ordered nanopores were preserved with the doping at the Eu 3+ molar concentration to Si up to 10mol%, and the O-Si-O and Si-OH groups in the structures were clearly rearranged with the doping, indicating the interaction of Eu 3+ with the O atoms. The significant morphological changes in the spheres were observed with the doping. The photoluminescence spectral shapes due to the transitions of 5D 0- 7F 1 and 5D 0- 7F 2 were indicative of the presence of the Eu 3+ in an environment of a low symmetry. It was found that the Eu 3+ was located inside the silica framework to electrostatically interact with the environmental O atoms, which would prevent the aggregation among Eu 3+ ions to show the efficient luminescence. Therefore, the interactions between the Eu 3+ ions and silica framework structures in the spheres were successfully clarified. © 2011 Elsevier Inc.

DOI： 10.1016/j.jcis.2011.07.066

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Efficient synthesis of Eu(III)-containing nanoporous silicas 査読有り

Tagaya M., Ikoma T., Yoshioka T., Motozuka S., Minami F., Tanaka J.

Materials Letters 65 ( 14 ) 2287 - 2290 2011年07月

記述言語：英語掲載種別：研究論文（学術雑誌）

Europium (III) (Eu3+)-containing nanoporous silicas were successfully synthesized by two different loading methods (adsorption or doping), and the states of the Eu3+ in the structure were investigated. The Eu3+-adsorption indicated that the Eu3+ interacts with hydroxyl groups on the pore surface and H2O molecules to enhance the quenching, whereas the Eu3+-doping indicated that the Eu3+ was located inside the structure framework that produced the efficient luminescence. The interaction between the Eu3+ and silica structure depended on the loading method. © 2011 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.matlet.2011.04.011

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Reaction between carbon dioxide and mechanically activated metal powder 査読有り

Nik N., Yokoyama S., Suzuki T., Motozuka S., Shimomura T., Sasano J., Izaki M.

Advanced Materials Research 129-131 799 - 803 2010年12月

記述言語：英語掲載種別：研究論文（国際会議プロシーディングス）

A fundamental study on the reaction between CO2 and mechanically activated metal powders has been conducted. In this research, the behavior and mechanism of CO2 reaction under various grinding conditions were investigated to fix and reduce CO2. The powder used was placed inside a grinding vessel, and was ground together with the SUJ2 balls in CO 2 atmosphere. It was found that only the adsorption of CO2 gas on the ground samples was observed, whereas the decomposition of CO 2 was not occurred. The CO2 adsorption increased proportionally with the increase in the grinding speed, weight of sample and number of SUJ2 balls. Furthermore, the CO2 adsorption increased with the decrease in the standard free energy of formation of each metal oxide. The morphology of the sample observed by SEM showed that the samples were not crushed into finer particles, but were only grazed on the sample's surface. Therefore, it can be said that the CO2 can be adsorbed on the mechanically activated samples by using the centrifugal type ball mill, but in order to enhance the amount of CO2 adsorption, another type of machine with higher grinding intensity should be considered. © (2010) Trans Tech Publications.

DOI： 10.4028/www.scientific.net/AMR.129-131.799

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