研究者詳細 - 荒井　規允

論文 - 荒井　規允

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最近の研究から「散逸粒子動力学シミュレーションによる両親媒性テトラポッド型ナノ粒子の自己集合制御」

荒木雄介, 荒井規允

アンサンブル（分子シミュレーション学会） 22 （ 1 ） 55 - 60 2020年

研究論文（研究会，シンポジウム資料等）, 査読有り, ISSN 1884-6750

近年，合成技術の発達によって様々な形状や表面を有すナノ粒子の作製が可能となった．そのようなナノ粒子は複雑な自己集合構造を示すことが報告されている．ナノ粒子の自己集合の制御や予測は，分子レベルからの機能性材料の設計に必要不可欠である．本研究では，両親媒性テトラポッド型ナノ粒子に着目し，腕の長さや親水/疎水比が自己集合へどのような影響を及ぼすか，散逸粒子動力学シミュレーションによって調べた．

Self-assembly of spheroidal triblock Janus nanoparticle solutions in nanotubes

Kobayashi Y., Inokuchi T., Nishimoto A., Arai N.

Molecular Systems Design and Engineering （Molecular Systems Design and Engineering） 4 （ 1 ） 122 - 132 2019年02月

研究論文（学術雑誌）, 共著, 査読有り, ISSN 2058-9689

© 2019 The Royal Society of Chemistry. We have performed coarse-grained molecular simulations to investigate the morphologies and phase diagrams of self-assembled spheroidal triblock Janus nanoparticles (JNPs) confined in nanotubes. Nanoparticles exhibit several unique behaviours through shape changes, such as high thermal conductivity in heat pipes, high strength of binding avidity in ligand-receptor interactions, high amounts of uptake between cells during endocytosis processes, and so on. In this study, we focus on the effect of shape on self-assembled structures or phases within nanospaces. We derived qualitative phase diagrams of axial pressure versus the ratio of the diameter of the nanoparticles and nanotubes. Two distinct types of nanotube walls and three types of JNP shapes were considered: hydrophobic and hydrophilic walls, and NP aspect ratios of 1.5, 2.0, and 2.5. We observed diverse morphologies in spheroidal JNP solutions, many of which have not been observed before in bulk solutions. We also compared the self-assembled structures of spherical triblock JNPs. By increasing the aspect ratio of the NPs, clusters of unique structures, such as tripods, tetrapods, and hexapods, were formed. Moreover, we found that an increase in the value of the aspect ratio leads to a shift in the multilayer toroidal stacking phases to a weaker confinement effect. The self-assembly behaviours of the spheroidal JNPs can be qualitatively predicted based on the chemical nature of the nanotube walls and shapes of the JNPs.

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Self-assembly of spheroidal triblock Janus nanoparticle solutions in nanotube

Y Kobayashi, T. Inokuchi, A. Nishimoto, N. Arai

Molecular Systems Design and Engineering 4 122 - 132 2019年02月

研究論文（学術雑誌）, 共著, 査読有り

Polymodal rheological behaviors induced by self-assembly of surfactants confined in nanotubes

Kobayashi Y., Arai N.

Journal of Molecular Liquids （Journal of Molecular Liquids） 274 328 - 337 2019年01月

研究論文（学術雑誌）, 単著, 査読有り, ISSN 01677322

© 2018 Elsevier B.V. Self-assembly is currently one of the most studied branches of materials chemistry, and has attracted a lot of attention due to its diverse potential applications in electronics, engineering, biomedical, and optical fields. Thus far, many previous studies have reported on the self-assembly of surfactants for developing various functional materials. In this study, we focus on the chemical nature of the wall surface as a critical parameter which can drastically change the self-assembled structure. We have studied the rheological properties of surfactant solutions in chemically distinct nanotubes using a computer simulation. Graphs of the Weissenberg number (Wi) versus the viscosity (η) in hydrophilic, hydroneutral, and hydrophobic nanotubes at different concentrations of surfactant were derived. We found that differences in the viscosity can be obtained depending on the chemical nature of the wall surface, even in systems without surfactant molecules. With the surfactant molecules, characteristic viscosity behaviors were observed with rich steady-state morphologies. For example, although the concentration of the surfactant is the same (c = 30%), completely different viscosity behaviors were observed in hydrophilic (shear-thinning) and hydrophobic (shear-thickening) nanotubes. Our simulations offer a guide to controlling the rheological properties of surfactant aqueous solutions by altering the chemical nature of the wall surface and elucidating the effects of confinement, the concentration of the surfactant aqueous solution, and the self-assembled structure.

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Polymorphic transitions mediated by surfactants in liquid crystal nanodroplet

Tsujinoue H., Inokuchi T., Arai N.

Liquid Crystals （Liquid Crystals） 46 （ 9 ） 1428 - 1439 2019年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 02678292

© 2019, © 2019 Informa UK Limited, trading as Taylor & Francis Group. Recently, various techniques have been developed using photonic crystals. Liquid crystals (LC) confined in a nanodroplet mimicked photonic crystals, such as those of opal. Therefore, investigating the phase behaviour of LC molecules in nanodroplets is very important in the next-generation optical field. In this study, the chemical interaction between surfactants and LCs in nanodroplets is reproduced using a dissipative particle dynamics method. We identify the phase behaviour of LCs and investigate how the chemical interaction affect on the orientation of LCs. In particular, by adding surfactant molecules, various morphological behaviours were observed in the LC nanodroplet. The phase transition temperature varied depending on RND (amount of surfactant molecules). Furthermore, difference of the self-assembly structure also appeared inside the droplet depending on RND. Our simulation offers a theoretical guide to control morphologies of self-assembled LCs inside a nanodroplet, a novel system that may find applications in nanofluidic devices or in photonic crystal technology.

Dissociation effect of non-covalent bond for morphological behavior of triblock copolymers: a dissipative particle dynamics study

Y Araki, N Arai

Chemical Engineering Communications, 1-13 （Chemical Engineering Communications） 208 （ 1 ） 1 - 13 2019年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 0098-6445

© 2019, © 2019 Taylor & Francis Group, LLC. The nanophase separation structure produced by block polymers is used for highly functional materials and has been studied for 50 years. In recent years, researchers have shown interest in introducing non-covalent bonds, such as hydrogen bonds and metal–ligand bonds, to polymers. The non-covalent bond dissociates or recombines in response to physical conditions, including temperature and concentration. The non-covalent bond freely controls the phase separation structure, namely, the physical properties of the polymer material. However, various interactions are involved in the formation process, for example, polymer–polymer, polymer–solvent, bonding and bending in the polymer. To control the self-assembled structure, it is necessary to understand the influence of the non-covalent bond at the molecular level. In this study, we investigated the effect of the non-covalent bond on a stage of phase separation immediately after dissociation (early-stage) of self-assembled morphologies by introducing the binding site to the triblock polymers. Various stable morphologies, including lamellar, lamellar with a grain boundary, and pre-lamellar, were observed by changing the positions of the non-covalent bond, their dissociation ratio, and the initial configurations. Moreover, we calculated the radial distribution function and static structure factor to identify the structural features. The results suggested that the early-stage of self-assembled morphology in polymer melt could be controlled by the position of the non-covalent bond and its dissociation ratio.

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Replica exchange dissipative particle dynamics method on threadlike micellar aqueous solutions

Y Kobayashi, K Nomura, T Kaneko, N Arai

Journal of Physics: Condensed Matter 32 (11), 115901 （Journal of Physics Condensed Matter） 32 （ 11 ） 115901 2019年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 0953-8984

© 2019 IOP Publishing Ltd. The self-assembly of surfactant molecules can spontaneously result in a variety of micelle morphologies, such as spherical micelles, threadlike micelles, and vesicles, and it is therefore crucial to predict and control the self-assembly to achieve a helpful process in the fields of materials chemistry and engineering. A dissipative particle dynamics (DPD) method used in a coarse-grained molecular simulation is applied to simulate various self-assembling soft matter systems because it can handle greater length and time scales than a typical molecular dynamics simulation (MD). It should be noted that the thorough sampling of a system is not assured at low temperatures because of large complex systems with coarse-grained representations. In this article, we demonstrate that the replica exchange method (REM) is very effective for even a DPD in which the energy barrier is comparatively lower than that of a MD. A replica exchange on DPD (REDPD) simulation for threadlike micellar aqueous solutions was conducted, and the values of the potential energy and the mean aggregation number were compared. As a result, the correct values and a self-assembled structure within a low-temperature range can only be obtained through the REDPD.

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Programmed self-assembly of tetrapod nanoparticles with an amphiphilic surface pattern: the effect of arm length and hydrophobic ratio

Y Araki, Y Kobayashi, N Arai

Molecular Systems Design & Engineering 4 (6), 1095-1102 （Molecular Systems Design and Engineering） 4 （ 6 ） 1095 - 1102 2019年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 2058-9689

© 2019 The Royal Society of Chemistry. We studied the self-assembly processes and morphologies of tetrapod nanoparticle solutions using dissipative particle dynamics (DPD) simulations. Composite-shaped nanoparticles, such as a tetrapod model with an amphiphilic surface pattern, were also synthesised experimentally. We programmed nanoparticle self-assembly using the DPD results at various values of the hydrophobic ratio (HR) and arm length (AL). Considering these two parameters, we observed the self-assembly processes and morphologies in a tetrapod nanoparticle solution. As a result, it was found that the HR and AL of tetrapod nanoparticles were effective parameters for controlling their self-assembly processes or structures under equilibrium. In this study, we programmed the AL or HR parameters, and we report their influences on self-assembly. Our simulations offer a guide to controlling the morphologies of self-assembled tetrapod nanoparticles, which constitute novel systems that may find applications in nanofluidic devices.

Predominant factor determining thermal conductivity behavior of nanofluid: Effect of cluster structures with various nanoparticles

Y Kobayashi, N Arai

Journal of The Electrochemical Society 166 (9), B3223-B3227 （Journal of the Electrochemical Society） 166 （ 9 ） B3223 - B3227 2019年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 0013-4651

© The Author(s) 2019. Despite several research efforts, the detailed mechanism that dominates the thermal conductivity of nanofluids has not been explained. We investigated the effect of the chemical surface design of NPs (hydrophobic–hydrophilic balance of the NPs containing Janus surface) and verified the influence of their self–assembled structures on the thermal conductivity of a nanofluid using molecular simulation. When hydrophobic (HO) NPs are added to a nanofluid, they only form one large cluster because they do not prefer to be in contact with water molecules. Hence, an increment in the thermal conductivity of the nanofluid added with HO NPs was observed. On the contrary, the mean cluster size of Janus NPs was limited because of their limited HO superficial areas (attractive domains). Hence, an increment in the enhancement ratio of thermal conductivity was not observed even when the volume fraction of the NPs (φNP) was increased. Thus, our results demonstrate that the mean cluster size of NPs is the key factor for thermal conductivity enhancement. In addition, this study reveals that it is possible to control the thermal conductivity of nanofluids (or the mean cluster size of Janus NPs) using Janus NPs with surfaces designed using anisotropic chemical interactions.

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Predicting molecular ordering in a binary liquid crystal using machine learning

T Inokuchi, R Okamoto, N Arai

Liquid Crystals, 1-11 （Liquid Crystals） 47 （ 3 ） 438 - 448 2019年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 0267-8292

© 2019, © 2019 Informa UK Limited, trading as Taylor & Francis Group. Machine learning is a category of AI technology that is utilized in the product development cycle in numerous industries. It was reported that machine learning can be applied to predict the chemical properties of functional materials, for example, the self-assembly of surfactant solutions (Nanoscale, 2018, 10, 16013) and the chemical reactions of copper nanoparticles (ACS Energy Lett., 2018, 3, 2983). A liquid crystal (LC) molecule is a representative functional material. Monodisperse systems have been targeted in many theoretical studies; however, the resulting products usually have a polydisperse distribution. It has been reported in several studies that the properties exhibited by polydisperse systems are different from those observed in monodisperse systems. In this study, we focus on the physical properties of polydisperse systems i.e. the ratio of binary LC molecules on the phase transition temperature and the possibility of predicting the physical properties of the system using machine learning. A relatively high prediction accuracy was obtained using machine learning. This study demonstrates that machine learning can be utilized to predict the phase transition temperature of polydispersed LC systems. The results of this study will contribute to the further development of material science and molecular design via the application of machine learning.

散逸粒子動力学（DPD）法を用いたソフトマターの分子シミュレーション

荒井規允

可視化情報学会誌（社団法人可視化情報学会） 39 （ 154 ） 19 - 25 2019年

研究論文（研究会，シンポジウム資料等）, 単著, 査読有り, ISSN 0916-4731

近年，コンピュータシミュレーション技術の発達によって，これまで取り扱うことのできなかった様々なシステムの再現，可視化が行われるようになってきた．散逸粒子動力学(DPD)法は分子シミュレーションの一種だが，原子や分子をある程度一纏めとして扱うことで，従来の分子シミュレーションよりも大きな時空間スケールの現象を再現できる．本稿では，DPD法の歴史，アルゴリズムを簡単に説明したあと，これまで筆者が対象としてきたいくつかのソフトマター材料(界面活性剤，ナノ粒子，液晶，高分子膜・生体膜)に対するDPDシミュレーションについて紹介する．

Water permeation in polymeric membranes: Mechanism and synthetic strategy for water-inhibiting functional polymers

Araki Y., Kobayashi Y., Kawaguchi T., Kaneko T., Arai N.

Journal of Membrane Science （Journal of Membrane Science） 564 184 - 192 2018年10月

研究論文（学術雑誌）, 単著, 査読有り, ISSN 03767388

© 2018 Elsevier B.V. The prediction and control of penetration in a polymeric membrane is of critical importance in green chemistry and energy technology, including gas separation, water purification, and desalination. We performed molecular simulations of water transport through a polymeric membrane to clarify the key factors that dominate water permeation. The effects of additives and chemical interaction (solubility) on water inhibition were investigated. We found that additives reduce water permeability into the membrane. Upon incorporation of the additive, strength of coordination of water molecules near the membrane surface increases. Thus, the penetration frequency of water molecules into the membrane decreases. It is suggested that the local environment near the membrane surface plays a significant role in controlling water permeability. In order to gain deeper insights into the polymer design, we discussed the chemical interaction (solubility) parameter change between polymer chains and additives. Using a repulsive chemical species of a polymer chain for additives can lead to higher water inhibition. The ability to control water permeability into the membrane by polymer design can be exploited for applications in water separation technology.

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Multiscale prediction of functional self-assembled materials using machine learning: High-performance surfactant molecules

Inokuchi T., Li N., Morohoshi K., Arai N.

Nanoscale （Nanoscale） 10 （ 34 ） 16013 - 16021 2018年09月

研究論文（学術雑誌）, 共著, 査読有り, ISSN 20403364

© 2018 The Royal Society of Chemistry. Various physical properties of functional materials can be induced by controlling their chemical molecular structures. Therefore, molecular design is crucial in the fields of engineering and materials science. With its remarkable development in various fields, machine learning combined with molecular simulation has recently been found to be effective at predicting the electronic structure of materials (Nat. Commun., 2017, 8, 872 and Nat. Commun., 2017, 8, 13890). However, previous studies have used similar microscale information as input and output data for machine learning, i.e., molecular structures and electronic structures. In this study, we determined whether multiscale data can be predicted using machine learning via a self-assembly functional material system. In particular, we investigated whether machine learning can be used to predict dispersion and viscosity, as the representative physical properties of a self-assembled surfactant solution, from the chemical molecular structures of a surfactant. The results showed that relatively accurate information on these physical properties can be predicted from the molecular structure, suggesting that machine learning can be used to predict multiscale systems, such as surfactant molecules, self-assembled micelle structures, and physical properties of solutions. The results of this study will aid in further development of the application of machine learning to materials science and molecular design.

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Self-assembled morphology of tripod nanoparticle solutions: the effect of arm length and hydrophobic ratio

Bin Sazali M., Kobayashi Y., Taniguchi Y., Nakashima T., Arai N.

Molecular Systems Design and Engineering （Molecular Systems Design and Engineering） 3 （ 3 ） 572 - 580 2018年06月

研究論文（学術雑誌）, 共著, 査読有り, ISSN 2058-9689

© 2018 The Royal Society of Chemistry. We have studied the self-assembled morphologies of tripod nanoparticle solutions confined in nanoslits using dissipative particle dynamics (DPD) simulations. In the present study, composite-shaped nanoparticles, like a planar tripod model with an amphiphilic surface pattern, were also synthesized experimentally. Using the DPD results at various values of a hydrophobic ratio (HR) and arm length (AL), we create phase diagrams of the self-assembled morphologies of tripod nanoparticles. With each of the two parameters, we observe three morphologies in the tripod nanoparticle solution. Further, potential energy vs. temperature for various tripod nanoparticle solutions is compared for different self-assembled structures. Our simulations offer a guide to control the morphologies of self-assembled tripod nanoparticles, which constitute novel systems that may find applications in nanofluidic devices.

Dissipative particle dynamics simulation of the relaxation behaviour of a triblock copolymer supramolecular network

Wakimoto K., Sasaki H., Arai N.

Molecular Simulation （Molecular Simulation） 44 （ 7 ） 534 - 539 2018年05月

研究論文（学術雑誌）, 単著, 査読有り, ISSN 08927022

© 2017 Informa UK Limited, trading as Taylor & Francis Group. Since block copolymers self-assemble into various nanostructures and these are widely used in soft materials such as cosmetics and paints, these continue to be the subjects of fundamental studies that progress new technologies. ABA triblock copolymers self-organise into supramolecular networks in which crosslinked structures change upon heating and other external stimulation. Supramolecular networks that consist of ABA triblock copolymers have three components: bridges, loops and dangles. These supramolecular networks have structural regions (clusters) in which end blocks of polymer chains are aggregated and connected by the internal blocks of the polymer chains. Despite of the importance of relaxation behaviour during the measurement and control of polymer materials, the molecular-level behaviour of these systems has not been addressed. We observed pull-out phenomenon that the ends of these polymers detach from clusters, and estimated characteristic detachment times by counting the number of detachments and compared it with the time of longest relaxation in that system.

Understanding a molecular motor walking along a microtubule: an asymmetric Brownian motor driven by bubble formation with a focus on binding affinity

Hojo M., Arai N., Ebisuzaki T.

Molecular Simulation （Molecular Simulation） 44 （ 7 ） 523 - 529 2018年05月

研究論文（学術雑誌）, 単著, 査読有り, ISSN 08927022

© 2017 Informa UK Limited, trading as Taylor & Francis Group. In recent years, many studies on a molecular motor have been conducted in the fields of biorheology and nanoengineering. The molecular motor is a molecule that converts the chemical energy obtained by ATP hydrolysis into mechanical energy. Explaining this mechanism is important for nanoengineering. A kinesin, which is a type of molecular motor, has the characteristics to move on a microtubule with hand-over-hand steps. The kinesin walking behaviour is explained by the ‘asymmetric Brownian ratchet model’. Previously, we had suggested that the walking mechanism was achieved by the bubble formation in a nanosized channel surrounded by hydrophobic atoms with the transition between the two states–bubble state and liquid state. However, the walking behaviour of the model motor was different from that of a single molecule measurement of a kinesin. In this study, we constructed a new motor system focused on the asymmetric binding affinity of a motor protein and performed a model simulation using the dissipative particle dynamics method. As a result, it was observed that hand-over-hand walking depends on the transition position ratio and the transition frequency coefficient. Moreover, the efficiency of the new motor system is higher than that of the previous motor systems. The new motor model can provide a simulation guide for the design of biomimetic nanomachines.

Self-assembly of peptide amphiphiles by vapor pressure osmometry and dissipative particle dynamics

Seki T., Arai N., Suh D., Ozawa T., Shimada T., Yasuoka K., Hotta A.

RSC Advances （RSC Advances） 8 （ 47 ） 26461 - 26468 2018年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 2046-2069

© The Royal Society of Chemistry. Peptide amphiphiles are one of the most promising materials in the biomedical field, so much effort has been devoted to characterizing the mechanism of their self-assembly and thermosensitive gelation. In this work, vapor pressure osmometry measurements were carried out to parameterize the thermosensitivity of interactions between peptide amphiphiles in an aqueous solution. The osmometry measurement verified that the peptides became more hydrophobic as temperature increased, which was quantitatively described with the Flory-Huggins χ parameter. Thereafter, a coarse-grained molecular model was used to simulate peptide amphiphiles dissolved in an aqueous solution. The temperature sensitive coarse-grained parameter aHW, which is the repulsive force between the hydrophilic head of the peptide amphiphile and water was estimated from the aforementioned experimentally obtained χ. Furthermore, the effects of concentration and temperature on the self-assembly behavior of peptide amphiphiles were quantitatively studied by dissipative particle dynamics. The simulation results revealed that aHW plays an important role in self-assembly characteristics and in the resulting microstructure of the peptide amphiphiles, which coincides with previous experimental and computational findings. The methodology in quantitatively linking the coarse-grained parameter from experiment and theory provides a sensible foundation for bridging future simulation studies with experimental work on macromolecules.

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Relationship between water permeation and flip-flop motion in a bilayer membrane

Inokuchi T., Arai N.

Physical Chemistry Chemical Physics （Physical Chemistry Chemical Physics） 20 （ 44 ） 28155 - 28161 2018年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 14639076

© 2018 the Owner Societies. The lipid bilayer membrane facilitates various biological reactions and is thus an essential structure that sustains all higher forms of life. The unique local environment of the lipid bilayer plays critical roles for the diffusion of biomolecules as well as water molecules in biological reactions. Although fluctuation of the cell membrane is expected to allow for the transport of some water molecules, the flip-flop of lipid molecules corresponds to lipid transport between membrane leaflets, and is considered to be an important process to regulate the lipid composition of biological membranes. However, the relationship between these flip-flop phenomena and surrounding water molecules remains poorly understood. We hypothesized that the flip-flop is caused by water molecules permeating through the cell membrane. To test this hypothesis, we used millisecond-order coarse-grained molecular simulations (dissipative particle dynamics) to investigate the distance between water molecules and lipid molecules depending on the position of the lipid molecule. The results clearly showed that water molecules affect the flip-flop motion in the early stage, but have minimal contribution to the subsequent behavior. Moreover, based on the results of dissipative particle dynamics simulation, we computed several first-passage-time (FPT) quantities to describe the detailed dynamics of water permeation. We modeled arrangements in the middle of the flip-flop process, which were compared with the arrangement without lipid molecules. Overall, our results indicate that lipid molecules located both in perpendicular and parallel arrangements largely affect water permeation. These findings provide new insight into the detailed relationship between water permeation and the flip-flop motion.

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Janus or homogeneous nanoparticle mediated self-assembly of polymer electrolyte fuel cell membranes

Kobayashi Y., Arai N.

RSC Advances （RSC Advances） 8 （ 33 ） 18568 - 18575 2018年

研究論文（学術雑誌）, 共著, 査読有り, ISSN 2046-2069

© 2018 The Royal Society of Chemistry. The functionality of polymer electrolyte fuel cell membranes depends on the self-assembled structure of the graft polymer. To control self-assembly, nanoparticles (NPs) are often used as catalysts. Hence, we investigate the effect of hydrophilic (HI), hydrophobic (HO), and Janus nanoparticles (JNPs) for the self-assembly of graft polymers using dissipative particle dynamics (DPD) simulations. We found that the differences that appeared among the self-assembled structures of water depended on the concentration of PEFC. We also calculated the diffusion constant of water (D(H2O)) from the slopes of the time-averaged mean square displacement (MSD) curves. HI NPs had the largest effect in suppressing the diffusion of water because the HI NPs incorporated into the water particles. It was also seen that D(H2O) with various NPs gradually decreased as the number of NPs increased for three PEFC concentrations (70%, 80%, and 90%). Thus, a close correlation between the position and chemical composition of NPs in polymer electrolyte fuel cell (PEFC) membrane systems has been found. Moreover, the mean square radius of gyration 〈Rg〉 and the mean square end-to-end distance 〈R〉 was calculated to analyse the self-assembled structures of PEFC. The 〈Rg〉 and 〈R〉 increased as the concentration of PEFC was increased, with and without various NPs.

Dissipative Particle Dynamics Simulation for Clarifying Mechanism of Water Permeation in Polymeric Membranes

Y Araki, N Arai, Y Kobayashi, T Kawaguchi, T Kaneko

Meeting Abstracts, 187-187 2018年

研究論文（国際会議プロシーディングス）, 共著, 査読有り

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