Article
Chemistry, Physical
Michael Lalanne-Tisne, Audrey Favrelle-Huret, Wim Thielemans, Joao P. Prates Ramalho, Philippe Zinck
Summary: Organocatalysts are important in polymerization reactions. This study used Density Functional Theory to investigate the ring-opening polymerization of trimethylene carbonate, revealing a dual mechanism and confirming TBD as a more efficient catalyst.
Article
Chemistry, Applied
Nicolas Zivic, Thomas Brossier, Floriane Crestey, Sylvain Catrouillet, Abraham Chemtob, Valerie Heroguez, Patrick Lacroix-Desmazes, Christine Joly-Duhamel, Sebastien Blanquer, Julien Pinaud
Summary: Patterned coatings based on biodegradable crosslinked poly(ester/carbonate) were prepared using photoinitiated ring-opening polymerization. The gel time was evaluated using photorheometry, and the formulation and experimental conditions were optimized for stereolithography to produce patterned coatings.
PROGRESS IN ORGANIC COATINGS
(2022)
Article
Polymer Science
Thomas Brossier, Gael Volpi, Vincent Lapinte, Sebastien Blanquer
Summary: The synthesis of semi-crystalline PTMC through ROP-amine shows promising results and compatibility with a variety of amines, offering a simple preparation method and the ability to monitor urethane bonds. The relationship between the nature of amines and the crystallinity of PTMC was discussed, along with the impact of crystallinity on the mechanical properties compared to amorphous PTMC.
Article
Polymer Science
Shuang Li, Han Lu, Ling Zhu, Meixue Yan, Xiaohui Kang, Yi Luo
Summary: The mechanisms of ring-opening polymerization of L-lactide and trimethylene carbonate using DMAP/Sac as a bifunctional catalyst were investigated using DFT calculations. A new two-component organocatalyst Adenine/Sac was also designed and evaluated for its catalytic performance. The results showed that Adenine/Sac exhibited higher catalytic activity in the ring-opening of L-lactide and trimethylene carbonate.
Article
Chemistry, Physical
Alexey Nikiforov, Natalia Panina, Daniil Blinou, Vladislav Gurzhiy, Juliya Nashchekina, Evgenia Korzhikova-Vlakh, Alexey Eremin, Mariia Stepanova
Summary: This study synthesized and studied carboxylate complexes of nickel(II) with different N-donor ligands for ring-opening polymerization (ROP) of lactide. Among the complexes, [Ni(DBED)(2)(O2CC(CH3)(3))(2)]center dot(CH3)(3)CCO2H showed the highest catalytic ability in the polymerization. A comprehensive density functional theory (DFT) study was conducted to understand the reaction mechanism and the role of carboxylate ligands in the process.
Article
Chemistry, Multidisciplinary
Dmitry S. Belov, Logesh Mathivathanan, Melanie J. Beazley, William Blake Martin, Konstantin V. Bukhryakov
Summary: The study explores the capability of an iron-based catalyst in performing ring-opening metathesis polymerization of olefins, demonstrating that the use of in situ prepared heteroleptic iron catalysts significantly enhances polymerization rate and selectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Polymer Science
Fabrice Azemar, Olinda Gimello, Julien Pinaud, Jean-Jacques Robin, Sophie Monge
Summary: This study reports the alcohol-free, ring-opening polymerization of trimethylene carbonate (TMC) in THF catalyzed by 1,5,7-triazabicyclo [4.4.0] ec-5-ene (TBD), producing PTMC with molecular weights up to 34,000 g/mol. The reaction proceeds rapidly with TBD catalysis in THF, yielding PTMC samples containing both linear and cyclic polymer chains.
Article
Polymer Science
Zhengyang Liu, Jinfeng Shi, Na Zhao, Zhibo Li
Summary: In this study, polysiloxanes with unique low temperature flexibility, including polydiethylsiloxane (PDES) and poly(dimethylsiloxane-co-diethylsiloxane) (PMES) copolymers, were successfully synthesized. The cyclic trimeric phosphazene base (CTPB) catalyzed ring-opening polymerization (ROP) at room temperature, resulting in high yields of PDES homopolymers with high molecular weights. Furthermore, the random copolymers of PMES with tunable diethylsiloxane contents were directly prepared via ring-opening copolymerization (ROCP) using CTPB as a catalyst. The controlled copolymer composition and the random distribution of diethylsiloxane and dimethylsiloxane units were confirmed by microstructure characterizations. The thermal property investigations demonstrated the good low-temperature flexibility and thermal stability of PMES copolymers, indicating their potential in extreme environmental applications.
EUROPEAN POLYMER JOURNAL
(2022)
Article
Polymer Science
Min Zhou, Zhemin Ji, Ximian Xiao, Longqiang Liu, Ruxin Cui, Zhengjie Luo, Zihao Cong, Runhui Liu
Summary: Poly(2-oxazoline)s are gaining increasing attention in the biomedical field due to their hydrophilicity and excellent biocompatibility. They can act as functional peptide mimics and potential substitutes for polyethylene glycol. Therefore, developing new polymerization methods for the synthesis of versatile poly(2-oxazoline)s is crucial. In this study, a controllable and facile synthesis of poly(2-oxazoline)s using trimethylsilyl trifluoromethanesulfonate (TMSOTf) as the initiator is reported. The polymerization exhibits temperature-dependent characteristics and allows for the synthesis of poly(2-oxazoline)s with desired chain length, various side chain functional groups, and narrow dispersities.
Review
Polymer Science
Dmytro Ryzhakov, Gael Printz, Beatrice Jacques, Samir Messaoudi, Francoise Dumas, Samuel Dagorne, Franck Le Bideau
Summary: Polyester synthesis through eco-friendly methods is a major challenge today, with metal complexes playing a crucial role as catalysts and initiators in the process. The use of metal-free organo-catalysts/initiators remains to be explored, with interesting developments reported over the past five years. This area of organo-catalyzed/initiated processes is still in its infancy but holds great potential for further advancements.
Article
Polymer Science
Rawan Omar, Muneer Shaik, Chloe Griggs, Jevin D. Jensen, Robert Boyd, Nuri Oncel, Dean C. Webster, Guodong Du
Summary: This study successfully synthesized a series of star-shaped poly (beta-hydroxybutyrates) (PHBs) through ring-opening polymerization of cyclic esters using multifunctional initiators, and characterized their structure and properties through various techniques. The thermal properties of star-shaped PHBs can be modified by changing the arm number and arm length, while the wetting behavior of star-shaped PHBs is influenced by the number of arms.
EUROPEAN POLYMER JOURNAL
(2021)
Article
Polymer Science
Chengliang Wang, Xu Zhang, Wei Zhao, Xin Liu, Qingfu Wang, Jingjiang Sun
Summary: This study introduces a novel organo-catalyzed method for the synthesis of hyperbranched aliphatic polycarbonates (HBPCs). The method allows for precise control over the HBPC structure and the introduction of different functional groups. HBPCs have significant potential for biomedical applications.
Article
Chemistry, Physical
Shaoqiao Li, Kairui Guo, Gong Chen, Jirong Wang, Yong Wang, Xingping Zhou, Zhigang Xue
Summary: Researchers have designed and synthesized a brush-typed polymer electrolyte with a structure that affects the performance of the electrolyte. The electrolyte, fabricated through a self-catalyzed strategy, exhibits excellent ionic conductivity and the ability to inhibit irregular lithium dendrite growth, providing a promising method for constructing high-performance ambient-temperature lithium metal batteries.
ENERGY STORAGE MATERIALS
(2022)
Article
Polymer Science
Oleksandr Ivanchenko, Ugo Authesserre, Guilhem Coste, Stephane Mazieres, Mathias Destarac, Simon Harrisson
Summary: ε-Thionocaprolactone (TCL) can be easily copolymerized with vinyl esters to form degradable copolymers, with the molecular weight and dispersity controlled through xanthate-mediated RAFT polymerization. Analysis of the copolymer structure reveals a high level of TCL-TCL dyads, suggesting that the terminal copolymerization model is not accurate for describing TCL copolymerization.
Article
Polymer Science
Siqi Li, Fangqin Song, Chuanhao Sun, Jieni Hu, Yan Zhang
Summary: The study reported the synthesis of a series of amphiphilic polymers with enhanced ROS-responsiveness through one-pot lipase-catalyzed polymerization, demonstrating that the selenide groups endowed nanoparticles with enhanced ROS-responsive properties, providing a potential material for further applications.
EUROPEAN POLYMER JOURNAL
(2021)
Article
Polymer Science
Huan Li, Yingying Li, Yudan Wang, Lijia Liu, Hongxing Dong, Chunhong Zhang, Toshifumi Satoh
Summary: Flexible and self-healing conductive hydrogel, called PVA/PDA/Tyr-PEAm, was developed to improve the antibacterial properties of electronic skin. The hydrogel exhibited long-term antibacterial activity, low hemolysis activity, good conductivity, and rapid self-healing ability. It could be used for detecting normal and wound skin in real-time, as well as detecting macro and micro movements of the human body.
EUROPEAN POLYMER JOURNAL
(2023)
Article
Polymer Science
Kai Chen, Chun -Yu Chen, Hsin-Lung Chen, Ryoya Komaki, Nao Kawakami, Takuya Isono, Toshifumi Satoh, Du -Yuan Hung, Ying-Ling Liu
Summary: This study reveals the strong effects of molecular architecture and configuration on the self-assembly behavior of sugar-based block copolymers. The configuration prescribed by the substituted positions of the block chains exerts a significant influence on the formation of hydrogen bonding and the resistance against bending. These findings provide insights into the controlled fabrication of ordered structures in green materials.
Article
Polymer Science
Xiaochao Xia, Tianle Gao, Feng Li, Ryota Suzuki, Takuya Isono, Toshifumi Satoh
Summary: Switchable polymerization has potential for synthesizing sequence-controlled macromolecules similar to natural biopolymers, but is limited to three-and four-component systems. We expanded its scope to five-component systems using a reactivity gradient among 12 monomers. Different copolymerizations were achieved using a catalyst, allowing for the synthesis of gradient and block copolymers. Anhydride reactivity was predicted using 13C NMR chemical shifts. This comonomer library allows for the prediction and preparation of more complex copolymer structures.
Article
Polymer Science
Huan Li, Yingying Li, Yudan Wang, Lijia Liu, Hongxing Dong, Chunhong Zhang, Toshifumi Satoh
Summary: In this study, a Lys-BPEA crosslinker was synthesized using primary amines rich in lysine end groups. An antibacterial self-healing hydrogel (PAA/Lys-BPEA) was prepared by introducing polyamine Lys-BPEA into PAA via ionic bonding and electrostatic interaction. The PAA/Lys-BPEA hydrogel exhibited excellent antibacterial and self-healing properties, making it an ideal choice for the design of smart self-healing devices and antibacterial surface coatings.
Article
Polymer Science
Ryohei Sato, Atsuo Utagawa, Koji Fushimi, Feng Li, Takuya Isono, Kenji Tajima, Toshifumi Satoh, Shin-ichiro Sato, Hiroshi Hirata, Yoshihiro Kikkawa, Takuya Yamamoto
Summary: The redox behaviors of macrocyclic molecules with an entirely pi-conjugated system were investigated in this study. Cyclic P3HT with different degrees of polymerization (DPn) were synthesized, and its unique redox behaviors were compared with linear P3HT. Cyclic P3HT showed a decrease in HOMO level and greater stability during cyclic voltammetry measurement, indicating stronger dicationic properties due to polaron-polaron interactions.
Article
Chemistry, Multidisciplinary
Erika Terada, Takuya Isono, Toshifumi Satoh, Takuya Yamamoto, Toyoji Kakuchi, Shinichiro Sato
Summary: Recently, temperature-responsive polymers tethered to oligooxyethylene side chains terminated with alkyl groups were experimentally investigated. Molecular dynamics simulations were used to study aqueous solutions of poly(glycidyl ether)s with different numbers of oxyethylene units. The thermal responses of chain extensions, hydrogen bond recombination, and water-solvation shells were analyzed. The phase-transition temperature was not directly related to the polymer-chain extensions, but the temperature response of the water-solvation shell around the alkyl group showed a noticeable correlation. The relationship between TCRP and TCLP was found to be affected by polymer-chain fluctuation.
Article
Chemistry, Multidisciplinary
Mahmoud M. Abd Elwakil, Ryota Suzuki, Alaa M. Khalifa, Rania M. Elshami, Takuya Isono, Yaser H. A. Elewa, Yusuke Sato, Takashi Nakamura, Toshifumi Satoh, Hideyoshi Harashima
Summary: mRNA lipid nanoparticles (LNPs) have been successfully developed to deliver mRNA to immune cells in the spleen, showing great potential for precision therapies. The design of ligand-free glycidylamine (GA) derivatives containing LNPs (GA-LNPs) with specific characteristics have significantly improved their self-assembly and RNA delivery efficiency. The top-performing estriol-GA05-30 LNPs exhibited strong antitumor activity and promising results in therapeutic and prophylactic cancer models, highlighting the importance of ionizable lipids for extrahepatic RNA delivery.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Minami Ebe, Asuka Soga, Kaiyu Fujiwara, Brian J. Ree, Hironori Marubayashi, Katsumi Hagita, Atsushi Imasaki, Miru Baba, Takuya Yamamoto, Kenji Tajima, Tetsuo Deguchi, Hiroshi Jinnai, Takuya Isono, Toshifumi Satoh
Summary: In this study, the synthesis of macro-rotaxanes consisting of high-molecular-weight axle and wheel components (macro-rotaxanes) was achieved by the topological trapping of multicyclic polydimethylsiloxanes (mc-PDMSs) in silicone networks. mc-PDMSs with more cyclic units and larger ring sizes can be quantitatively trapped in the network as macro-rotaxanes, compared to monocyclic PDMS. The damping performance of a 60 wt % mc-PDMS-blended silicone network was found to be higher than the bare PDMS network, suggesting the potential application of macro-rotaxanes as non-leaching additives for network polymers.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Feng Li, Ryota Suzuki, Tianle Gao, Xiaochao Xia, Takuya Isono, Toshifumi Satoh
Summary: Polymer materials are crucial in shaping modern society. The development of new catalysts, such as alkali metal carboxylates, plays an important role in the continuous advancement of polymer materials. These simple compounds have demonstrated their potential as catalysts in various polymerization reactions.
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
(2023)
Article
Chemistry, Applied
Satoshi Katsuhara, Naoki Sunagawa, Kiyohiko Igarashi, Yutaka Takeuchi, Kenji Takahashi, Takuya Yamamoto, Feng Li, Kenji Tajima, Takuya Isono, Toshifumi Satoh
Summary: This study synthesized cellulose acetate-based TPEs with different degrees of substitution (DS) and investigated the impact of DS on their structure and properties. The results showed that decreasing DS led to the formation of a more ordered microphase-separated structure, improved toughness, suppressed stress relaxation, and enhanced biodegradability potential. This work demonstrates the potential of cellulose acetate-based TPEs as next-generation sustainable materials.
CARBOHYDRATE POLYMERS
(2023)
Article
Chemistry, Physical
Yuanyuan Gu, Lijia Liu, Yudan Wang, Chunhong Zhang, Toshifumi Satoh
Summary: Hierarchical chiral self-assembly of an amphiphilic helical poly(phe-nylacetylene) homopolymer containing bi-valine pendants was achieved by adding a polar solvent into the polymer solution. The influences of solvent components and temperature on the supramolecular chirality and morphologies of ordered nanostructures were investigated. Various morphologies including spheres, beads-string micelles, vesicles, nanorods, flower-like, and blocky nanostructures were obtained. The chiral property endowed by bi-valine pendants in the polyphenylacetylene backbone was transferred and enhanced in high-ordered supramolecular self-assemblies. The increase of polar solvent fraction significantly promoted the aggregation of multi micelles.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Multidisciplinary
Hien Thi Phan, Shoko Furukawa, Koto Imai, Hiroya Tomita, Takuya Isono, Toshifumi Satoh, Ken'ichiro Matsumoto
Summary: Bacterial polyhydroxyalkanoate (PHA) synthase PhaC(AR) and its mutated variants were used to synthesize block copolymers with poly(d-lactate) (PDLA) segments. Beneficial mutations N149D and F314H increased the incorporation of D-lactate (LA) units, resulting in the synthesis of P(3HB)-b-PDLA and P(3HHx)-b-PDLA. This study demonstrates a new method for the synthesis of block copolyesters with isotactic PDLA segments from renewable resources using engineered polyester synthase.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Polymer Science
Yamato Ebii, Yoshinobu Mato, Feng Li, Kenji Tajima, Takuya Yamamoto, Takuya Isono, Toshifumi Satoh
Summary: In this study, multicyclic polystyrene (mc-PS) was successfully synthesized through the cyclopolymerization of alpha,omega-dinorbornenyl end-functionalized PS macromonomers mediated by the Grubbs third-generation catalyst. The number of cyclic units in the obtained mc-PS was controlled by adjusting the macromonomer-to-G3 ratio, with a maximum of 239 units achieved. The developed cyclopolymerization strategy provides a new approach for the synthesis of multicyclic polymers and has significant implications for fundamental studies and material applications.
