Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

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Language：English   Publishing type：Research paper (scientific journal)  

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.biomaterials.2020.120162

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

We report the preparation of tough, thermally stable, and water-resistant double-network (DN) ion gels, which consist of a partially-clustered silica nanoparticle network and poly(ionic liquid) (PIL) network holding an ionic liquid. Silica nanoparticles/poly([Evim][Tf2N]) DN ion gels are prepared by photo-induced radical polymerisation of [Evim][Tf2N] in a mixture containing silica nanoparticles, [Bmim][Tf2N], ionic liquid based cross-linker [(VIM)(2)C-4][Tf2N](2), and ethyl acetate, followed by subsequent solvent evaporation. Tensile strength measurements show that the mechanical properties of the PIL DN ion gels were higher than those of the PIL single-network (SN) ion gel. A rheological study indicates that an enhancement in mechanical strength of the PIL DN ion gels can be achieved when silica nanoparticles form partial clusters in [Bmim][Tf2N]. The cyclic stress-strain measurement of the PIL DN ion gels shows hysteresis loops, suggesting that the silica nanoparticle clusters rupture and dissipate the loading energy when the PIL DN ion gels undergo a large deformation. The fracture strength and Young's modulus of the PIL DN ion gels increase as the diameter of the silica nanoparticles is decreased. Thermogravimetric analysis measurement shows that the PIL DN ion gel has a high decomposition temperature of approximately 400 degrees C. Moreover, the swelling test shows that the PIL DN ion gel possesses an excellent water-resistant property because of the hydrophobic nature of the PIL backbone. We believe that such tough, thermally stable, and water-resistant PIL DN ion gels can be used as carbon dioxide separation membranes, sensors, and actuators for soft robotics.

DOI： 10.1039/c9sm02213a

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

We report a simple process to fabricate monodisperse tetra-arm poly(ethylene glycol) (tetra-PEG) hydrogel microcapsules with an aqueous core and a semipermeable hydrogel shell through the formation of aqueous two-phase system (ATPS) droplets consisting of a dextran-rich core and a tetra-PEG macromonomer-rich shell, followed by a spontaneous cross-end coupling reaction of tetra-PEG macromonomers in the shell. Different from conventional techniques, this process enables for the continuous production of hydrogel microcapsules from water-in-oil emulsion droplets under mild conditions in the absence of radical initiators and external stimuli such as heating and ultraviolet light irradiation. We find that rapid cross-end coupling reaction of tetra-PEG macromonomers in ATPS droplets in the range of pH from 7.4 to 7.8 gives hydrogel microcapsules with a kinetically arrested core-shell structure. The diameter and core-shell ratio of the microcapsules can be easily controlled by adjusting flow rates and ATPS compositions. On the other hand, the slow cross-end coupling reaction of tetra-PEG macromonomers in ATPS droplets at pH 7.0 and lower induces structural change from core-shell to Janus during the reaction, which eventually forms hydrogel microparticles with a thermodynamically stable crescent structure. We believe that these hydrogel microparticles with controlled structures can be used in biomedical fields such as cell encapsulation, biosensors, and drug delivery carriers for sensitive biomolecules.

DOI： 10.1021/acs.langmuir.8b04169

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DOI： 10.1107/S1600576718007264

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

We report the controlled formation of internally porous polyelectrolyte particles with diameters ranging from tens to hundreds of micrometers through selective solvent extraction using microfluidics. Solvent-resistant microdevices, fabricated by frontal photopolymerization, encapsulate binary polymer (P)/solvent (Si) mixtures by a carrier solvent phase (C) to form plugs with well-defined radii and low polydispersity; the suspension is then brought into contact with a selective extraction solvent (S2) that is miscible with C and Si but not P, leading to the extraction of Si from the droplets. The ensuing phase inversion yields polymer capsules with a smooth surface but highly porous internal structure. Depending on the liquid extraction time scale, this stage can be carried out in situ, within the chip, or ex situ, in an external S2 bath. Bimodal polymer plugs are achieved using asymmetrically inverted T junctions. For this demonstration, we form sodium poly(styrenesulfonate) (P) particles using water (S1), hexadecane (C), and methyl ethyl ketone (S2). We measure droplet extraction rates as a function of drop size and polymer concentration and propose a simple scaling model to guide particle formation. We find that the extraction time required to form particles from liquid droplets does not depend on the initial polymer concentration but is rather proportional to the initial droplet size. The resulting particle size follows a linear relationship with the initial droplet size for all polymer concentrations, allowing for the precise control of particle size. The internal particle porous structure exhibits a polymer density gradient ranging from a dense surface skin toward an essentially hollow core. Average particle porosities between 10 and 50% are achieved by varying the initial droplet compositions up to IS wt % polymer. Such particles have potential applications in functional, optical, and coating materials.

DOI： 10.1021/la404506b

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Publishing type：Research paper (international conference proceedings)   Publisher：Japan Society of Mechanical Engineers  

DOI： 10.1299/jsmermd.2021.1p2-k05

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

<p>Clickable ionic liquid monomers realize the one-pot synthesis of ionically conducting poly(ionic liquid)s with 1,2,3-triazolium-based backbones<italic>via</italic>click chemistry.</p>

DOI： 10.1039/d0ra07948k

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

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Publishing type：Research paper (scientific journal)   Publisher：The Japanese Society for Multiphase Flow  

DOI： 10.3811/jjmf.2020.t007

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Language：English   Publishing type：Research paper (scientific journal)  

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

A flow process for the production of poly(methyl methacrylate) (PMMA) particles is proposed by soap-free emulsion polymerization using a water-in-oil (W/O) slug flow in a microreactor. Thin oil films generated around the dispersed aqueous phase of the W/O slug prevent the prepared particles from adhesion to the microchannel wall, enabling the continuous production of PMMA particles without clogging. The effects of the linear flow rate of the slug flow and the addition of ethanol in the dispersed aqueous phase on the polymerization are evaluated. It is found that increasing the linear flow rate of the slug flow or the addition of ethanol in the dispersed aqueous phase results in PMMA particles with high molecular weight (approximate to 1500 kg mol(-1)) in 20 min reaction time. It is believed that this process would be a promising way to prepare polymer particles with high molecular weight in a short reaction time.

DOI： 10.1002/macp.201900021

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

We report a simple preparation of free-standing metal films via electroless plating (ELP) at the liquid-liquid (L-L) interface between an aqueous electroless plating solution and an organic solvent. The use of ELP does not require any external energy in the form of heating and stirring. We find that the affinity of the organic solvent for the palladium nanoparticles (PdNPs) as catalysts and the vertical position of the organic and aqueous phases in the biphasic system are important considerations for synthesizing a robust copper film. Specifically, 1,2-dichloroethane which has an appropriate affinity for PdNPs and a higher density than water was found to be a good candidate for use as the organic phase in this system. However, a poor-quality copper film was obtained in the system with 1-hexanol as the organic phase. We also controlled the microscale surface structure of the copper films by using different concentrations of the injected PdNP dispersion. A high density of PdNPs caused smaller regions of metal growth, which contributed to the formation of smoother metal films. Moreover, under the optimal synthesis condition, we confirmed the electrical conductivity of the obtained copper film to be 1.16 X 10(-7) Omega m. We believe that this metal film preparation represents a promising way to produce a range of metal film structures through the use of flexible L-L interfaces as templates.

DOI： 10.1021/acs.langmuir.8b02822

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

Nature creates beautiful structural colors, and some of these colors are produced by nanostructural arrays of melanin. Polydopamine (PDA), an artificial black polymer produced by self-oxidative polymerization of dopamine, has attracted extensive attention because of its unique properties. PDA is a melanin-like material, and recent studies have reported that photonic materials based on PDA particles showed structural colors by enhancing color saturation through the absorption of scattered light. Herein, we describe the preparation of three-dimensional (3D) colloidal photonic materials, such as structural color balls and fibers, from biomimetic core shell particles with melanin-like PDA shell layers. Structural color balls were prepared through the combined use of membrane emulsion and heating. We also demonstrated the use of microfluidic emulsification and solvent diffusion for the fabrication of structural color fibers. The obtained 3D colloidal materials, i.e., balls and fibers, exhibited angle-independent structural colors due to the amorphous assembly of PDA-containing particles. These findings provide new insight for the development of dye-free technology for the coloration of various 3D colloidal architectures.

DOI： 10.1021/acsami.7b03453

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE BV  

Reverse micelles are thermodynamically stable systems, with a capacity to encapsulate hydrophilic molecules in their nanosized core, which is smaller than the core generally obtained with water in -oil-emulsion droplets. Herein, we present a simple technique for the preparation of poly(ethylene glycol)-block-polylactide (PEG-b-PLA) nanocapsules encapsulating a hydrophilic photosensitizer (indocyanine green, ICG), which exploits reverse micelle formation and subsequent emulsion-solvent diffusion. We establish the effect of the PEG-b-PLA composition and the co-surfactant volume on the diameter and water content of the reverse micelles. We demonstrate that the composition of PEG-b-PIA affects also the diameter and encapsulation efficiency of the resulting nanocapsules. We show that the ICG-laden nanocapsulescon fabricated under the most optimal conditions have a diameter of approximately 100 nm and an ICG encapsulation efficiency of 58%. We believe that the method proposed here is a promising step towards the preparation of hydrophilic drug-laden polymer nanocapsules with a small diameter and therefore suitable for use in drug delivery applications based on enhanced permeability and retention (EPR) effect-driven passive targeting. (C) 2017 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.colsurfa.2017.02.039

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Authorship：Lead author   Language：English   Publishing type：Research paper (international conference proceedings)   Publisher：IEEE  

This conference proceeding reports a preliminary result regarding a simple technique to fabricate core-shell tetra-arm poly(ethylene glycol) (tetra-PEG) hydrogel microbeads encapsulating insulin-secreting cells using microfluidic emulsification and interfacial coupling reaction of two kinds of tetra-PEG macromonomers at the core-shell interface in the precursor aqueous droplets. Different from conventional PEG-based microbeads formation, in situ gelation system utilizing self-diffusion of the macromonomers in confined microdroplets allowed to prepare tetra-PEG hydrogel microbeads with narrow size distribution under mild gelation condition in the absence of heating and UV irradiation. This technology can be used to generate monodisperse tetra-PEG hydrogel microbeads to encapsulate sensitive cells for regenerative medicines.

DOI： 10.1109/MEMSYS.2016.7421728

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE BV  

The effects of photo-triggered tumor vascular treatment (PVT) on the structural and functional properties of tumor vasculature were assessed in Colon-26 (C26) and B16/BL6 (B16) tumor-bearing mice. Furthermore, anti-tumor efficacy of subsequently injected PEG liposomal paclitaxel (PL-PTX) was also evaluated. As a photosensitizer, a hydrophobic porphyrin derivative was used and formulated in polymeric nanoparticle composed of polyethylene glycol-block-polylactic acid to avoid its non-specific in vivo disposition. In the mice bearing C26 with high permeable vasculature, the prominent anti-tumor activity was confirmed by PVT alone, but the subsequently injected PL-PTX did not show any additive effect. PVT itself initially induced apoptotic cell death of tumor vascular endothelial cells and platelet aggregation, which would have subsequently induced apoptosis of C26 tumor cells surrounding the vasculature. On the other hand, in the mice bearing B16 with low permeable vasculature, PVT enhanced the anti-tumor activity of subsequently injected PL-PTX, which would be attributed to the tumor disposition amount and area of PEG liposomes enhanced by PVT. These results clearly indicated that the treatment would have made it possible to provide more efficient extravasation of PL-PTX, leading to its more potent anti-tumor effect. (C) 2015 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.jconrel.2014.12.038

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：NATURE PUBLISHING GROUP  

Understanding and engineering the flow-response of complex and non-Newtonian fluids at a molecular level is a key challenge for their practical utilisation. Here we demonstrate the coupling of microfluidics with small angle neutron scattering (SANS). Microdevices with high neutron transmission (up to 98%), low scattering background (less than or similar to 10(-2) cm(-1)), broad solvent compatibility and high pressure tolerance (approximate to 3-15 bar) are rapidly prototyped via frontal photo polymerisation. Scattering from single microchannels of widths down to 60 mu m, with beam footprint of 500 mu m diameter, was successfully obtained in the scattering vector range 0.01-0.3 angstrom(-1), corresponding to real space dimensions of similar or equal to 10-600 angstrom. We demonstrate our approach by investigating the molecular re-orientation and alignment underpinning the flow response of two model complex fluids, namely cetyl trimethylammonium chloride/pentanol/D2O and sodium lauryl sulfate/octanol/brine lamellar systems. Finally, we assess the applicability and outlook of microfluidic-SANS for high-throughput and flow processing studies, with emphasis of soft matter.

DOI： 10.1038/srep07727

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Publishing type：Research paper (international conference proceedings)  

This paper describes the preparation of insulin secreting (MIN6m9) cell-laden calcium alginate (Ca-Alg) hydrogel microfiber coated with poly-L-ornithine (PLO) using a microfluidic wet-spinning, followed by layer-by-layer (LbL) deposition to enhance the mechanical strength. Both in vitro and in vivo experiments showed that PLO-coated (PLO-Alg) microfiber had higher mechanical strength than Ca-Alg microfiber. In addition, the cells encapsulated in PLO-Alg microfiber after 7 days of culture secreted insulin in response to glucose concentrations. We believe that PLO-Alg microfiber can be useful for the application in robust tissue graft to achieve long-term implantation.

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

A simple approach to preparing monodisperse poly(D, L-lactide) (PDLLA) microcapsules with a single aqueous core is developed. The method is based on automatic water-in-oil-in-water double emulsion formation from oil-in-water single emulsion via spontaneous emulsification which voluntarily disperses part of continuous aqueous phase into the dispersed oil phase dissolving oil-soluble amphiphilic diblock copolymer, poly(D, L-lactide)-b-poly(2-dimethylaminoethyl methacylate)(PDLLA-b-PDMAEMA), followed by coalescence of tiny water droplets within the polymer droplets, coupled with quick precipitation of polymers by diluting the emulsion with water. In this study, we have investigated the effect of PDLLA to PDLLA-b-PDMAEMA ratios and flow rates of each solution during preparing the emulsion on the final morphology and the size of the microcapsules. It was found that the polymer blend ratio played a crucial role in determining internal structure of the microcapsules. The microcapsules size decreased with the increment of the flow rate ratios of the continuous phase to the dispersed phase and eventually reached 10 mm, while maintaining narrow size distribution. In addition, we have demonstrated that the microcapsules can encapsulate both hydrophilic and hydrophobic compounds during the formation.

DOI： 10.1039/c3ra44066d

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

We describe a versatile and facile route to the continuous production of monodisperse polylactide (PLA) microcapsules with controllable structures. With the combination of microfluidic emulsification, solvent diffusion, and internal phase separation, uniform PLA microcapsules with a perfluorooctyl bromide (PFOB) core were successfully obtained by simply diluting monodisperse ethyl acetate (EA)-in-water emulsion with pure water. Rapid extraction of EA from the droplets into the aqueous phase enabled the solidification of the polymer droplets in a nonequilibrium state during internal phase separation between a concentrated PLA/EA phase and a PFOB phase. Higher-molecular-weight PLA generated structural complexity of the microcapsules, yielding core-shell microcapsules with covered with small PFOB droplets. Removal of the PFOB via freeze drying gave hollow microcapsules with dimpled surfaces. The core-shell ratios and the diameter of these microcapsules could be finely tuned by just adjusting the concentration of PFOB and flow rates on emulsification, respectively. These biocompatible microcapsules with controllable size and structures are potentially applicable in biomedical fields such as drug delivery carriers of many functional molecules.

DOI： 10.1021/la403883a

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：PHARMACEUTICAL SOC JAPAN  

To develop potent paclitaxel (PTX) formulations for cancer chemotherapy, we formulated PTX into polymeric nanoparticles composed of polyethylene glycol (PEG) and polylactic acid (PLA) block copolymer (PN-PTX). First, the physicochemical properties of PN-PTX prepared were assessed; the mean particle size was around 80nm and the zeta potential was found to be almost neutral. Next, the in vitro PTX release property was assessed by a dialysis method. Although rapid release of PTX was observed just after dosing, around 70% of PTX was stably incorporated in polymeric nanoparticles for a long time in the presence of serum. Then, the in vivo pharmacokinetics of PN-PTX after intravenous administration was investigated in Colon-26 (C26) tumor-bearing mice. Both polymeric nanoparticles and PTX incorporated exhibited a long blood circulating property, leading to enhanced permeability and retention (EPR) effect-driven, time-dependent tumor disposition of PTX. Tumor distribution increased gradually for 24h, and tissue uptake clearance of polymeric nanoparticles in the liver and spleen was lower than that of PEG liposomes. Since these results indicated that the in vivo disposition characteristics of PN-PTX were very favorable, we then evaluated the anti-tumor effect of PN-PTX in C26 tumor-bearing mice. However, PN-PTX did not exhibit any significant anti-tumor effect, presumably due to the poor PTX release from polymeric nanoparticles. From these results, it is considered that the favorable pharmacokinetic properties of nanoparticles and the drug incorporated do not always lead to its potent in vivo pharmacological activity, suggesting the importance of PTX release properties within tumor tissues.

DOI： 10.1248/bpb.b12-0020

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Monodisperse polylactide (PLA) microspheres were continuously fabricated by microfluidic emulsification and subsequent dilution in water. The diameter was precisely tuned from 6 to 50 mu m by changing the flow rate of the fluids in microfluidics or the PLA concentration in the dispersed phase. The use of amphiphilic oil-soluble poly(ethylene glycol)-b-polylactide (o-PEG-PLA) as a matrix resulted in a highly porous microsphere morphology, and the porosity was controlled by blending PLA. Therefore, mono-disperse PLA microspheres with the predetermined surface porosity were continuously produced by just enough reagents and energy.

DOI： 10.1039/c1sm05910f

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Language：Japanese   Publisher：(一社)日本糖尿病学会  

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Language：English   Presentation type：Oral presentation (general)  

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Language：English   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：English   Presentation type：Oral presentation (general)  

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Language：English   Presentation type：Symposium, workshop panel (nominated)  

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Language：English   Presentation type：Poster presentation  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：English   Presentation type：Poster presentation  

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Language：English   Presentation type：Poster presentation  

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Language：English   Presentation type：Poster presentation  

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Language：English   Presentation type：Poster presentation  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Poster presentation  

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Language：Japanese   Presentation type：Poster presentation  

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Language：English   Presentation type：Poster presentation  

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Language：English   Presentation type：Poster presentation  

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Language：English   Presentation type：Poster presentation  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Poster presentation  

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Language：Japanese   Presentation type：Poster presentation  

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Language：English   Presentation type：Poster presentation  

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Language：English   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：Japanese   Presentation type：Oral presentation (general)  

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Language：English   Presentation type：Poster presentation  

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Application no：特願2019-014565  Date applied：2019.1.30

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Application no：特願2016-221135  Date applied：2016.11.14

Announcement no：特開2018-078917  Date announced：2018.5.24

Patent/Registration no：特許第6935896号  Date registered：2021.8.30 

Rights holder：竹内昌治;興津輝;渡邉貴一;小沢文智;長田翔伍

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Author：Myself 

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Author：Other 

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Author：Myself 

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Author：Myself 

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Author：Other 

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