研究者詳細 - 金岡　鐘局

論文 - 金岡　鐘局

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Multiarm Star-Crosslinked Hydrogel: Polymer Network with Thermoresponsive Free-End Chains Densely Connected to Crosslinking Points 招待査読国際誌

Shohei Ida*, Shogo Toda, Masatoshi Oyama, Hiroki Takeshita, Shokyoku Kanaoka*

Macromolecular Rapid Communication 42 ( 8 ) 2000558 2021年4月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Wiley 参加形態：共同（主担当）

Soft tissue in biological system is a hydrogel with elaborate structure exhibiting repeatable dynamic function. In order to approach such sophisticated system, precise construction of a designed network with multi‐components is desired. This communication presents a novel hydrogel having highly dense stimuli‐responsive free‐end chains around crosslinking structure. A key molecule is a core‐crosslinked star‐shaped polymer with multiple thermoresponsive arms, which can be prepared by reversible addition–fragmentation chain transfer polymerization of divinyl crosslinker with poly(N‐isopropylacrylamide) (PNIPAAm) macro‐chain transfer agent and have a number of unreacted carbon–carbon double bonds in the core. These unreacted double bonds can be utilized as a crosslinker for poly(acrylamide) (PAAm) gel synthesis by free radical polymerization. The obtained gel contains homogeneously dispersed star PNIPAAms as crosslinking points and exhibits thermoresponsive swelling behavior in water depending on the star contents. In particular, the gel with low content of the star crosslinker shows localized responsive behavior with expansion and shrinkage of the star in one molecule. The mechanical properties of the star‐crosslinked gel are significantly high compared to the conventional PAAm gels particularly in compressive strength (≈9 MPa). Moreover, the star‐crosslinked gel has thermoresponsive mechanical toughening property.

DOI： 10.1002/marc.202000558

その他リンク： https://onlinelibrary.wiley.com/doi/10.1002/marc.202000558

Facile synthesis of macroscopic bilayer gels by one-shot radical polymerization in phase-separated binary solvent systems 招待招待査読国際誌

Shohei Ida*, Ryuto Soma, Iori Ono, Takumitsu Kida, Shokyoku Kanaoka*

Polymer Journal accepted 2025年

Facile synthesis of acrylamide derivative copolymers with side urethane groups for systematic variation of the thermoresponsive behavior 査読国際誌

Shohei Ida*, Ryu Hashiguchi, Yusuke Murai, Kaito Nakamura, Kazuki Yano, Shokyoku Kanaoka*

Polymer Journal 56 ( 8 ) 735 - 743 2024年8月

Solution Properties of Amphiphilic Alternating Copolymers of N-Ethylmaleimide and 2-Hydroxyethyl Vinyl Ether: Thermoresponsiveness in Alcohols and Cosolvency Phenomenon in Binary Ethanol/Water Solutions 査読国際誌

Kaito Nakamura, Kazuki Yano, Shohei Ida*, Daichi Ida*, Akiyuki Ryoki, Shunichiro Yamamoto, Takaya Terashima, Shokyoku Kanaoka*

Macromolecules 57 ( 9 ) 4439 - 4447 2024年5月

Temperature-Induced Nanostructure Formation Behavior of Core Cross-Linked Star-Shaped Poly(N-isopropylacrylamide) in Water 査読

Ken Terao*, Masahiro Abe, Masafumi Nagase, Sayuri Takeshima, Shohei Ida, and Shokyoku Kanaoka*

Macromolecules 56 ( 14 ) 5635 - 5641 2023年7月

Thermoresponsive “Irreversible” Property Change of POSS-Crosslinked PNIPAAm Hydrogels 招待査読

Shohei Ida*, Tenki Hikida, Atsumi Kawai, Tomonari Matsuda, Souma Suzuki, Hiroaki Imoto, Kensuke Naka, Shokyoku Kanaoka*

Polymer Chemistry 14 ( 23 ) 2771 - 2778 2023年6月

Structure–property correlation of crosslinked domain hydrogels exhibiting thermoresponsive mechanical toughening and hybridization with photoluminescent carbon dots 査読

Shohei Ida, Takahiro Okuno, Miki Morimura, Kazumasa Suzuki, Hiroki Takeshita, Masatoshi Oyama, Keiji Nakajima, Shokyoku Kanaoka

Polymer Chemistry 13 ( 23 ) 3479 - 3488 2022年6月

pH-responsive aggregation control of multiarm star polymers depending on the ionic segment sequence of arm polymers 査読

Kitajima H., Ida S., Bhowmik S., Yusa S.i., Kanaoka S.

Polymer Journal 2022年1月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Polymer Journal

A deep understanding of the effect of the ionic density in a polymer on the solution properties would contribute to the development of novel stimuli-responsive materials. To this end, a multibranched and highly dense structure is an attractive platform for the accumulation of ionizable groups. In this study, we focus on core-crosslinked multiarm star polymers having ionizable poly(acrylic acid) (PAA) segments in the arms with different sequences to evaluate the density effect of ionic segments on pH-responsive properties. Two types of star polymers with a PAA block on the outer or inner side of an arm chain in combination with a hydrophilic poly(2-hydroxyethyl acrylate) (PHEA) block were synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization. These star polymers exhibited aggregation behavior different from the corresponding linear block polymer in an acidic aqueous solution. Dynamic light scattering analysis in water revealed that the star polymer with PAA in the outer layer formed larger aggregates than the star polymer with the inverse layer structure, and the pH-responsive change of the hydrodynamic radius in water depends on the sequence in the arm polymers. This behavior resulted from the balance of hydrogen bonding between PAA and PHEA segments and PAA electrostatic repulsion.

DOI： 10.1038/s41428-022-00621-3

Scopus

その他リンク： https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85124735390&origin=inward

Thermoresponsive Property of Polymer Hydrogels Induced by Copolymerization of Hydrophilic and Hydrophobic Monomers: Comprehensive Study from Monomer Sequence and Water Affinity 査読国際誌

Shohei Ida*, Daiki Nishisako, Ayaka Fujiseki, Shokyoku Kanaoka*

Soft Matter 17 ( 25 ) 6063 - 6072 2021年7月

Design of Hydrogels with Thermoresponsive Crosslinked Domain Structures via the Polymerization-Induced Self-Assembly Process and Their Thermoresponsive Toughening in Air 査読国際誌

Morimura M., Ida S., Oyama M., Takeshita H., Kanaoka S.

Macromolecules 54 ( 4 ) 1732 - 1741 2021年2月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Macromolecules 参加形態：共同（副担当）

We designed a hydrogel with a thermoresponsive crosslinked domain (CD) structure, which expressed thermoresponsive toughening in an isochoric manner in air. The responsive behavior of conventional thermoresponsive hydrogels is usually a macroscopic volume change along with water transfer to and from the outside of the polymer network. In order to expand the scope of thermoresponsive hydrogels, a network design that requires no external water for thermoresponsive transition has been demanded. To this end, we focused on the polymerization-induced self-assembly process for the direct synthesis of gels with designed domains and performed reversible addition-fragmentation chain transfer polymerization of N-isopropylacrylamide in water at a high temperature using a bifunctional macro-chain transfer agent, yielding a transparent gel. The structural analysis of the obtained gel revealed that dispersed CDs reversibly swelled and shrunk in response to temperature change in air without aggregation. Such an internal structural change induced the increase of elastic modulus and elongation at a high temperature.

DOI： 10.1021/acs.macromol.0c02569

Scopus

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pH- and thermo-responsive behavior of PNIPAM star containing terminal carboxy groups in aqueous solutions 査読国際誌

Sharker K.K., Takeshima S., Toyama Y., Ida S., Kanaoka S., Yusa S.

Polymer 203 122735 2020年7月

Supramolecularly Designed Thermoresponsive Polymers in Different Polymer Backbones 査読

Naya M., Kokado K., Landenberger K., Kanaoka S., Aoshima S., Sada K.

Macromolecular Chemistry and Physics 2020年1月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Macromolecular Chemistry and Physics

© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Thermoresponsive polymers in water, for example, poly(N-isopropylacrylamide) (PNIPAM) are investigated extensively, due to a wide range of biomedical applications. However, the attempts to control thermoresponsiveness are still rare in less or nonpolar media. Herein, the three thermoresponsive homopolymers tethering an N-butylurea group in the side chain with a different polymer backbone are reported. They exhibit lower critical solution temperature (LCST)-type and upper critical solution temperature (UCST)-type thermoresponsiveness depending on association of the urea group in the polymer chain and hydrogen bonding small molecules (effectors) in ternary systems (polymer/effector/organic solvent). The difference of polymer backbone appears as their change of solvophobicity in organic solvents. Poly(methacrylate) backbone needs more amount of the effector in nonpolar organic solvents, and poly(vinyl ether) backbone needs more amount in polar organic solvents. However, the influence of polymer backbone is too little to change the phase transition behavior, and the thermoresponsiveness is dominated by association and dissociation of hydrogen bondings between polymers and effectors. The supramolecular design of the thermoresponsive polymers is strong and extensible for the design of their phase transitions.

DOI： 10.1002/macp.201900455

Scopus

その他リンク： https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85078658476&origin=inward

Thermoresponsive core cross-linked star-shaped poly(N-isopropylacrylamide) for reversible and controlled aggregation of nanoscale molecular units 査読国際誌

Ida S., Toyama Y., Takeshima S., Kanaoka S.

Polymer Journal 2019年11月

Swelling and mechanical properties of thermoresponsive/hydrophilic conetworks with crosslinked domain structures prepared from various triblock precursors 査読国際誌

Ida S., Morimura M., Kitanaka H., Hirokawa Y., Kanaoka S.

Polymer Chemistry 10 ( 45 ) 6122 - 6130 2019年10月

Facile one‐shot synthesis of functional star‐shaped polymers by domino‐type living cationic copolymerization 査読国際誌

Mayuka Yamada, Arihiro Kanazawa, Shokyoku Kanaoka, Sadahito Aoshima

Journal of Polymer Science: Part A, Polymer Chemistry 57 ( 21 ) 2166 - 2174 2019年9月

Dual stimuli-responsive copolymers with precisely arranged degradable units: Synthesis by controlled alternating copolymerization of oxyethylene-containing vinyl ethers and conjugated aldehydes 査読

Matsumoto S., Kanazawa A., Kanaoka S., Aoshima S.

Polymer Chemistry 10 ( 30 ) 4134 - 4141 2019年8月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Polymer Chemistry 参加形態：共同（副担当）

© 2019 The Royal Society of Chemistry. Thermoresponsive alternating, block, and gradient-like copolymers with acid-degradability were synthesized via controlled cationic copolymerization of conjugated aldehydes and vinyl ethers (VEs). The thermoresponsive behavior of the resultant copolymers in water was governed by the polymer sequence. For example, an alternating copolymer was soluble in water at low temperature and displayed a sharp one-step phase separation on heating. By contrast, a block copolymer consisting of a degradable alternating sequence and a VE homosequence exhibited two-step phase separation in water. The alternating copolymers contained acid-labile acetal linkages in the main chain at periodic intervals and thus decomposed rapidly into small molecules without residual oligomers under acidic conditions. The block and gradient-like copolymers were hydrolyzed into VE polymers and oligomers, respectively, due to the presence of non-degradable VE-VE linkages. The thermoresponsive patterns of the hydrolysis products differed from those of the original polymers.

DOI： 10.1039/c9py00513g

Scopus

その他リンク： https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85070230787&origin=inward

Screening of metal complex catalysts using bidentate Schiff base ligands for controlled cationic polymerization of vinyl ethers using: In situ complexation method 査読

Kigoshi S., Kanazawa A., Kanaoka S., Aoshima S.

Polymer Chemistry 10 ( 30 ) 4209 - 4219 2019年8月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Polymer Chemistry 参加形態：共同（副担当）

© 2019 The Royal Society of Chemistry. Various ligands were screened for the cationic polymerization of isobutyl vinyl ether (IBVE) via in situ complexation using ZrCl4 as a catalyst precursor. [N,O]-Type phenoxyimine ligand frameworks were found to be more efficient for controlled polymerization compared to ligands that coordinate to the metal via two oxygen ([O,O]-type ligands) or two nitrogen ([N,N]-type ligands) atoms. In particular, the N-aryl phenoxyimine ligand with tBu groups on the phenol moiety was effective in terms of the controllability of the polymerization, catalyst solubility, catalytic activity, and ease of derivatization. Moreover, optimization of reaction conditions led to the expansion of the applicable metal species for controlled cationic polymerization. The polymerization of IBVE using the N-phenyl phenoxyimine ligand/TiCl4 initiating system in the absence of ethyl acetate in toluene at -78 °C produced a well-controlled polymer. In addition, the phenoxyimine/ZrCl4 systems were effective for the controlled polymerization of various monomers including St derivatives. The easily tunable electronic properties were also useful for the controlled bulk polymerization.

DOI： 10.1039/c9py00351g

Scopus

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Biomineralization-inspired fabrication of chitosan/calcium carbonates core-shell type composite microparticles as a drug carrier 査読

Tanimoto S., Nishii I., Kanaoka S.

International Journal of Biological Macromolecules 129 659 - 664 2019年5月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：International Journal of Biological Macromolecules 参加形態：共同（副担当）

© 2019 Elsevier B.V. Chitosan/calcium carbonate core-shell type composite microparticles were fabricated via a biomineralization-inspired process with chitosan particles as starting materials. The obtained composite particles were spherical, and the diameter of the composite particles was larger than that of the chitosan particles. XRD measurement indicated that the shell of the composite particle had a crystalline structure. The shell fabrication process was carried out with polyacrylic acid (PAA) or polyglutamic acid (PGlu) as binder molecules between calcium carbonate and chitosan. The crystal form of the shell fabricated with PAA was calcite, which is the most stable form of calcium carbonate crystal. On the other hand, the shell fabricated with PGlu was composed mainly with vaterite crystal, which is not a stable form. Types of the binder molecules influenced the crystal structure of the calcium carbonate shell. Drug release behavior of the model drug-introduced core-shell particles was evaluated in various pH conditions. It was revealed that the inorganic shell suppressed drug release and that the crystal form of the calcium carbonate shell affected suppression of drug release. The core-shell particles prepared in this study was an environmentally friendly hybrid product consisting of inorganic and organic materials and could be used as a novel drug-carrying microcapsule.

DOI： 10.1016/j.ijbiomac.2019.02.063

Scopus

その他リンク： https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85061558790&origin=inward

Controlled Cationic Polymerization of 1-Methoxy-1,3-Butadiene: Long-Lived Species-Mediated Reaction and Control over Microstructure with Weak Lewis Bases 査読

Togo Y., Kanazawa A., Kanaoka S., Aoshima S.

Journal of Polymer Science, Part A: Polymer Chemistry 57 ( 3 ) 288 - 296 2019年2月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Polymer Science, Part A: Polymer Chemistry 参加形態：共同（副担当）

© 2018 Wiley Periodicals, Inc. Controlled cationic polymerization of trans-1-methoxy-1,3-butadiene was achieved through the design of appropriate initiating systems, yielding soluble polymers with controllable molecular weights. The combined use of SnCl4 or GaCl3 as a Lewis acid catalyst and a weak Lewis base in conjunction with HCl as a protonogen resulted in efficient and controlled polymerization. The Mn values of the product polymers increased linearly along the theoretical line, which indicates that intermolecular crosslinking reactions negligibly occurred. In addition, the polymer microstructure was critically dependent on the weak Lewis base employed. In particular, the use of tetrahydrofuran as an additive resulted in the highest 4,1/4,3-structure ratio (96/4). Weak Lewis bases also affected the polymerization rates but exhibited unique trends that differed from their effects on the cationic polymerization of alkyl vinyl ethers. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 288–296.

DOI： 10.1002/pola.29090

Scopus

その他リンク： https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85053039781&origin=inward

Tetradentate Schiff Base Ligand/MCl <inf>n</inf> Initiating Systems for the Controlled Cationic Polymerization of Isobutyl Vinyl Ether: Effects of the Ligand Framework 査読

Kigoshi S., Kanazawa A., Kanaoka S., Aoshima S.

Journal of Polymer Science, Part A: Polymer Chemistry 2019年1月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Polymer Science, Part A: Polymer Chemistry 参加形態：共同（副担当）

© 2019 Wiley Periodicals, Inc. We investigated the cationic polymerization of vinyl ethers using metal complex catalysts with salen and salphen ligands. Metal complexes were generated in situ from the reaction of a ligand and a metal chloride. The choice of a ligand and a central metal was crucial for tuning the catalyst function such as catalytic activity and controllability of the polymerization. Among metal chlorides employed, ZrCl 4 was the most efficient for controlled polymerization. Cationic polymerization of isobutyl vinyl ether (IBVE) proceeded using the salen and salphen-type ligand/ZrCl 4 initiating systems, yielding polymers with predetermined molecular weights and narrow molecular weight distributions. Importantly, the structural effects of the complex catalysts were responsible for the polymerization behavior. For example, the polymerization using the salen-type ligand/ZrCl 4 system was much slower than that using the salphen-type ligand/ZrCl 4 system. In addition, the polymerization of IBVE using the salen-type ligand/FeCl 3 system proceeded in a controlled manner, which was in contrast to uncontrolled polymerization using the salphen-type ligand/FeCl 3 system. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019.

DOI： 10.1002/pola.29354

Scopus

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