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  • We demonstrated biomolecular motors driven swarming of microtubules and their dissociation under UV and visible light irradiation, respectively. A photoresponsive molecule, para tert-butyl-substituted azobenzene was incorporated to the backbone of single strand DNA, which functions as a photoswitch to control the swarming of microtubules in a reversible manner. This work is expected to expand the potential applications of biomolecular motors in developing photoregulated molecular machines.

    • Satsuki Ishii
    • Mousumi Akter
    • Akira Kakugo
    Rapid Communication
  • This review focuses on the controlled radical polymerization of vinyl ether (VE) and the related self-assemblies. VE was long believed to be among the monomers that could not be radically homopolymerized. Under such circumstances, some groundbreaking polymerizations of VE have been discovered. Advances in research have made it possible to perform controlled radical polymerization with VE due to hydrogen bonds and/or cation-π interactions between VE monomers and the propagating radical. By using the resulting poly(VE)s, various functional polymers and nano-objects via polymerization-induced self-assembly can be obtained.

    • Shinji Sugihara
    Focus Review
  • P3HT embedded with N- and NS-GQDs exhibit quite similar crystallinities independently of the solvent used, as suggested by our molecular dynamics calculations for the amorphous and crystalline regions. The vibrational, optical and impedance spectroscopy features suggest charge carrier formation in both the amorphous and crystalline regions but only for the P3HT:NS-GQDs system in relation to the donor:acceptor interactions evidenced by our DFT calculations.

    • Dominique Mombrú
    • Mariano Romero
    • Álvaro W. Mombrú
    Original Article
  • This focus review discussed our recent developments of unnatural glycopolymers based on polyoxazoline, protein–polymer conjugates, and protein stabilization. To develop new glycopolymers, a bicyclic monomer composed of glucosamine and 2-methyl-2-oxazoline (MeOx) was designed. This cationic ring-opening polymerization proceeded not by the mechanism for MeOx but by a new polymerization mechanism. This oligosaccharide has promise to be applied to a new glycomaterial owing to the polymer design. Additionally, protein conjugation and encapsulation by amphiphilic/fluorous chain-folding nanoparticles were investigated. Fluorous nature in random copolymers was useful for the protein conjugation and stabilization.

    • Yuta Koda
    Focus Review
  • The lithium halides; LiBr, LiCl, and LiI were well dispersed in the PMMA matrix. The pinning effects of the PMMA chains due to the addition of the salts were enhanced in the viscoelastic spectra with increasing as the anion sizes. Moreover, it was suggested from the Griffith Theory, the stress concentration around the salts in the PMMA matrix acts as the crack initiation.

    • Asae Ito
    • Arisa Shin
    • Koh-hei Nitta
    Original Article
  • The polymer chain morphologies of poly(4-iodostyrene) (P4IS) adsorbed on gold nanoparticles (GNPs) inside a polystyrene matrix were visualized using annular dark-field scanning transmission electron microscopy. The P4IS polymer chains adsorbed on GNPs exhibited a unique morphology wherein 1–2 molecular layers of P4IS surrounded a GNP, and the rest of the P4IS was aggregated at the side of the GNP. Enthalpy gain for the surrounding layer via adsorption and entropy gain for the remaining polymer chains via aggregation was considered the reason why the morphology was preferred.

    • Tomohiro Miyata
    • Yoshiaki Kawagoe
    • Hiroshi Jinnai
    Original Article
  • The drug release behaviors of gelatin hydrogels prepared with polymers in terms of their rheological properties were evaluated. In the oscillatory strain sweep, gelatin/HPMCP hydrogels showed a higher crossover strain (Tan δ = 1) than gelatin and gelatin/Eudragit® hydrogels. Thus, gelatin/HPMCP hydrogels had the property of elastic hydrocolloids and tended to keep the platform compared with other sample hydrogels. As a result, the drug release from gelatin/HPMCP hydrogels was delayed compared with other sample hydrogels at pH 1.2.

    • Satoshi Nogami
    • Kazunori Kadota
    • Yuichi Tozuka
    Original Article
  • The first ultrasoft aqueous lithium-ion batteries with coaxial fiber structures were fabricated with an all-hydrogel design. The all-hydrogel fiber aqueous Li-ion battery exhibited a high specific discharge capacity of 84.8 mAh·g−1 and superior cycling behavior and rate capacity performance. A low Young’s modulus (e.g., 445 kPa) for the battery was achieved by making it entirely from hydrogels, which ensured mechanical compatibility with biological tissues.

    • Jiacheng Wang
    • Tingting Ye
    • Ye Zhang
    Rapid Communication
  • Viscoelastic properties of comb-shaped ring (RC) polystyrenes with different branch chain lengths were investigated. Even for the RC sample with short branches, a plateau of the dynamic modulus G*(ω) was observed, suggesting the intermolecular branch chain entanglement occurred. In the region between the plateau and terminal regions, G*(ω) was observed with a weaker angular frequency dependence than the terminal relaxation. The G*(ω) data were analyzed with two models: the comb-Rouse model, in which the structures of RC molecules are taken into account by graph theory, and the Milner-McLeish model for entangled star-shaped polymers.

    • Yuya Doi
    • Jinya Kitamura
    • Yushu Matsushita
    Original Article
  • Among stimuli-responsive polymers, thermoresponsive poly(N-isopropylacrylamide) (PNIPAAm) is the most widely investigated. PNIPAAm-based polymers can undergo appropriate changes in response to their external environment. In this focus review, recent advancements in the applications of stimuli-responsive polymers based on PNIPAAm in biomedical fields are summarized, with an emphasis on our own research. In particular, a summary of the design of polymers for application in the separation and purification of (bio)pharmaceutical products and controlled cellular uptake is provided.

    • Yuki Hiruta
    Focus Review
  • The liquid-phase exfoliation of graphite is mass-producible and cost-effective method of graphene production. Polymers can be employed as dispersants to facilitate the exfoliation of graphite in organic solvents. We synthesized methacrylate polymers with various monomer ratios and molecular weights and investigated the efficient acquisition of graphene from graphite. Graphene with a uniform thickness was obtained when graphite was exfoliated using an optimized polymer dispersant.

    • Shimpei Takeda
    • Yuta Nishina
    Rapid Communication
  • The crystalline phase and phase transition behavior of an optically transparent film of star-shaped (heptaisobutyl-T8-silsesquioxy)propyl-substituted octadimethylsiloxy-Q8-silsesquioxane (star-POSS) were studied by DSC and WAXS measurements. This star-POSS exhibited a crystalline phase with a hexagonal system at room temperature and underwent melting above the melting temperature (Tm). The specimens underwent recrystallization even at temperature above Tm, resulting in the same hexagonal system with slightly larger a- and c-axis lengths. The amorphous state of the surrounding isobutyl substituents on the T8-cage framework provides an optically transparent film.

    • Rina Suzuki
    • Lina Li
    • Kensuke Naka
    Original Article
  • We report the nonradiative decay dynamics of charge transfer (CT) states generated in nonfullerene-acceptor-based polymer solar cells. The nonradiative decay rate constants knr decreased with an increase in the efficiency for dissociation of CT states into free carriers, indicating that nonradiative decay of CT states can be mitigated by increasing the delocalization of the CT state wave function.

    • Shin-ichiro Natsuda
    • Toshiharu Saito
    • Yasunari Tamai
    Original Article
  • Asymmetric combinations of chiral 2-hydroxyalkanoic acid (2HAA)-based random copolymers with monomer compositions of approximately 50/50, which can form stereocomplex (SC) crystallites, are reported. The copolymer combinations were l-configured individually crystallizable poly(l-lactic acid-co-l-2-hydroxybutanoic acid) or poly(l-2-hydroxybutanoic acid-co-l-2-hydroxy-3-methylbutanoic acid) and d-configured individually noncrystallizable poly(d-lactic acid-co-d-2-hydroxy-3-methylbutanoic acid). This study strongly suggests that SC crystallization occurred when the common monomer units were incorporated into both l- and d-configured 2HAA-based random copolymers. SC crystallization of new types of asymmetric combinations is expected to diversify the attainable properties and biodegradation behavior of chiral 2HAA-based polymer materials.

    • Hideto Tsuji
    • Katsuya Osanai
    • Yuki Arakawa
    Original Article
  • This review is focused on evolutions of precision radical polymerizations in various directions from metal-catalyzed Kharasch addition or atom transfer radical addition (ATRA). The developments include metal-catalyzed living radical polymerizations via reversible activation of carbon-halogen bonds, metal-catalyzed step-growth radical polymerizations of designed monomers having an unconjugated vinyl group and a reactive carbon-halogen bond, simultaneous metal-catalyzed chain- and step-growth radical polymerization for producing degradable vinyl copolymers with main-chain ester units, and vinyl monomer sequence control via combinations of iterative ATRAs and various controlled polymerizations.

    • Masami Kamigaito
  • Hetero-telechelic poly(ethylene glycol)s that contain a hydroxy group and a maleimide-furan adduct their α and ω ends, respectively, were isolated as a novel type of hetero-telechelic polymers (HTPs) via the post-modification of commercially available hydroxy-terminated PEGs with furan-protected p-maleimidophenyl isocyanate and subsequent purification with reversed-phase column chromatography at critical conditions.

    • Tatsuki Sato
    • Rikito Takashima
    • Hideyuki Otsuka
    Original Article
  • We report a thermally cross-linkable fluorescent polymer and its assembly to insoluble microbeads by hydrothermal annealing. A novel fluorene-based poly(triarylamine) bearing crosslinkable styryl groups on a fluorene unit is newly designed and synthesized by a Pd-catalyzed amination reaction. The polymer self-assembles into spherical microparticles and becomes insoluble to organic solvents by hydrothermal crosslinking without losing the spherical morphology. Mixing of the polymer with polystyrene enhances the photoluminescence quantum yield by suppressing the aggregation induced quenching and induces a spectral shift of the emission band to green and red after annealing.

    • Yuta Ihara
    • Hiroshi Yamagishi
    • Yohei Yamamoto
    Original Article
  • The addition of rGO affected the molecular and crystalline structures of electrospun PLLA scaffolds, leading to the enhanced piezoresponse. An increase of rGO content up to 1 wt% resulted in the increased number of polar C=O functional groups at the surface of fibers and degree of crystallinity of scaffolds. The maximum increase of the effective local lateral piezoresponse (13.9 pm/V) was achieved for 0.2 wt% rGO doping, which is explained by the presence of the shear piezoelectric α-phase (P212121) in uniaxially oriented PLLA fibers and C=O bond rotation in the polymer chains.

    • Igor O. Pariy
    • Roman V. Chernozem
    • Roman A. Surmenev
    Original Article