Article
Materials Science, Multidisciplinary
Alexander Joseph Cunningham, Xiantao Feng, Hu Zhang, Xavier Banquy, Jeanne Leblond Chain, Xiao-Xia Zhu
Summary: This study investigates the thermoresponsive properties of block copolymers based on a bile acid, finding that the PEG length and amine groups play a role in the LCST behavior.
MATERIALS TODAY COMMUNICATIONS
(2021)
Review
Polymer Science
Bo Pang, Yuewen Yu, Wangqing Zhang
Summary: In recent years, significant progress has been made in the research of thermoresponsive polymers based on tertiary amine moieties, which exhibit unique phase transition properties in aqueous solutions and can be modulated by the solution's pH value and CO2.
MACROMOLECULAR RAPID COMMUNICATIONS
(2021)
Article
Polymer Science
Lu Lian, Qingqing Wang, Fujin Duan, Youliang Zhao
Summary: Rational macromolecular design can enable polymers to exhibit thermoresponsive behaviors according to specific requirements. By synthesizing poly(amido thioether)s with different side groups, it is possible to achieve single or dual phase transitions that are concentration-independent, exhibit good thermal stability, and show both UCST and LCST behaviors.
Article
Chemistry, Applied
Sarah Otto, Paula Facal Marina, Fiona Zhou, Anton Blencowe
Summary: This study successfully converted non-responsive polysaccharides into thermoresponsive polysaccharides with tuneable lower-critical solution temperatures (LCSTs) by functionalising dextran with alkylamide groups. The newly developed alkylamide-functionalised dextrans exhibited good solubility and tunable LCSTs, showing potential for biomedical applications such as drug-delivery.
CARBOHYDRATE POLYMERS
(2021)
Article
Materials Science, Multidisciplinary
Bo-Yuan Chuang, Chun-Yao Ke, Yu-Jen Shao, Ken-Tsung Wong, Guey-Sheng Liou
Summary: Polyarylamine-based dielectric electrets and pentacene as p-type semiconductors were used to fabricate photoresponsive flash transistor memories. The PDTPmC electret, with high dipole moment, coplanar conformation, and highly conjugated structure, demonstrated outstanding hole-trapping capability and photorecoverability. The PDTPmC-based memory device exhibited excellent switching reliability and readout current ratio.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Saqib Kamal, Arif I. Inamdar, Kuan-Ru Chiou, Batjargal Sainbileg, Muhammad Usman, Jenq-Wei Chen, Tzuoo-Tsair Luo, Michitoshi Hayashi, Chen-Hsiung Hung, Wen-Feng Liaw, Kuang-Lieh Lu
Summary: This study investigated the effects of different functional groups on the dielectric behavior of coordination polymers. The results showed that electron-donating and electron-withdrawing groups altered the polarity of the polymers, which in turn affected the dielectric constant. Theoretical calculations supported the experimental findings and revealed distinct electronic behaviors and wide bandgaps in these compounds. This study provides important information for further research on the effects of different functional groups on the dielectric properties of coordination polymers.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Gregorio Guzman-Gonzalez, Soline Vauthier, Marta Alvarez-Tirado, Stephane Cotte, Laurent Castro, Aurelie Gueguen, Nerea Casado, David Mecerreyes
Summary: A family of single-ion lithium conducting polymer electrolytes based on highly delocalized borate groups has been reported, with the effect of substituents on boron atom analyzed. The polymer with flexible and electron-withdrawing substituents demonstrates the highest ionic conductivity among reported lithium single-ion conducting homopolymers. Combining high lithium transference number and good electrochemical stability, it shows promise for application in lithium batteries.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Shaon Dey, Arpita Roy, Kalipada Manna, Sagar Pal
Summary: A hydrogen bonded UCST polymer has been developed by grafting of methacrylamide and acrylic acid on dextran via free radical polymerization. The copolymer forms H-bonds between acid and amide groups at low temperature, making it insoluble in water. It becomes soluble beyond a certain temperature when the H-bonds collapse. The effects of pH, monomer composition, and polymer and salt concentration on the cloud point have been explored.
Article
Chemistry, Inorganic & Nuclear
Yan-Bing Wang, Chenlong Nan, Weize Zhuo, Chen Zou, Hui Jiang, Xin-Qi Hao, Changle Chen, Mao-Ping Song
Summary: The introduction of O-donor groups on amine-imine ligands leads to the synthesis of a series of nickel complexes, which exhibit high catalytic activities and produce polyethylene elastomers with high molecular weight. Moreover, these nickel complexes can also catalyze the copolymerization of ethylene with various functional monomers to prepare functionalized polyolefins.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Shuangshuang Hou, Jiarui Hu, Xueting Liang, Daohong Zhang, Bien Tan
Summary: The study focused on the simple and efficient preparation of porous hyper-cross-linked polymers (HCPs) using low-cost carbonates as building blocks, resulting in functional polymers with high gas adsorption performance and selectivity. Fine-tuning the molecular structure of the building blocks allowed for rational tuning of the texture property and gas capturing capacity of the obtained polymers, providing insight into structure-property relationships.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Polymer Science
Natalia Smigiel-Gac, Anna Smola-Dmochowska, Henryk Janeczek, Piotr Dobrzynski
Summary: The article presents the synthesis and characteristics of amphiphilic block terpolymers consisting of a hydrophilic polyesteramine block and hydrophobic blocks made of lactidyl and glycolidyl units. These terpolymers were obtained through copolymerization of L-lactide with glycolide using macroinitiators with protected amine and hydroxyl groups. The terpolymers were designed to have biodegradability, biocompatibility, antibacterial properties, and high surface wettability by water. The properties of the terpolymers, such as molecular mass, contact angle, crystallinity, and melting behavior, were evaluated using various tests.
Article
Polymer Science
Haobo Yuan, Takumitsu Kida, Yuma Ishitobi, Ryo Tanaka, Masayuki Yamaguchi, Yuushou Nakayama, Takeshi Shiono
Summary: The copolymerization of norbornene and fluorene-containing alkene comonomers using the Me2Si(Flu)((NBu)-Bu-t)-TiMe2 complex as a catalyst resulted in copolymers with high activity and gradient structure. Dynamic mechanical analysis showed phase separation of the copolymer, confirming the formation of the gradient structure. The obtained copolymers exhibited high refractive index and extremely low photoelasticity.
Article
Chemistry, Multidisciplinary
Sabrina S. Scott, Brahmjot Kaur, Cameron H. M. Zheng, Patrick Brant, Damon J. Gilmour, Laurel L. Schafer
Summary: Early transition metal-catalyzed hydroamino-alkylation is an efficient method to add amines to polybutadienes, offering access to amine-functionalized polyolefins. Tantalum catalyst can be used to functionalize different ratios of 1,2-polybutadiene polymers, and the degree of amination can be controlled by modifying amine and catalyst loading.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Boyang Huang, Pengbin Lai, Haiming Hua, Ruiyang Li, Xiu Shen, Xueying Yang, Peng Zhang, Jinbao Zhao
Summary: In this paper, a low molecular weight polyether poly (EO-co-PCGE) (PECP) is synthesized and blended with PEO-based solid polymer electrolyte (SPE) to improve its ionic conductivity. The introduction of low molecular weight and cyclic carbonate pendant in the PEO matrix reduces crystallinity and affects the conduction mechanism, significantly increasing the lithium-ion transference number. The prepared PEO-based SPE exhibits excellent ionic conduction properties, especially at room temperature, and enables LiFePO4/Li batteries to have excellent cycling performance at 40 degrees C.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Multidisciplinary
Ilker Torun, Conan Huang, Mustafa Kalay, Moonsub Shim, M. Serdar Onses
Summary: This article introduces the pH tunable assembly of quantum dots (QDs) over functional patterns prepared by electrohydrodynamic jet printing of poly(2-vinylpyridine). The pH of the dispersion provides tunability at two levels, allowing for modulation of QDs adsorption density and fluorescence. The selective adsorption of QDs enables both deterministic patterning and hierarchically structured encoding of information. Through image analysis and feature matching algorithms, it is demonstrated that these patterns are unclonable and suitable for anti-counterfeiting applications.
Article
Chemistry, Multidisciplinary
Robert D. Murphy, Ronnie V. Garcia, Seung J. Oh, Tanner J. Wood, Kyoo D. Jo, Javier Read de Alaniz, Ed Perkins, Craig J. Hawker
Summary: Describes the synthesis of functional hydrogels from 3-arm diblock copolypeptide stars, which achieve mechanical stability and biological activity through physical and photo-crosslinking, enabling direct ink writing of 3D objects with high precision and biological viability.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Kwangho Yoo, Gue Seon Lee, Hyo Won Lee, Byeong-Su Kim, Jeung Gon Kim
Summary: Mechanochemistry has been successfully applied to polymer synthesis, achieving efficiency, greenness, and new products. In this study, solid monomers were reacted with secondary butyl lithium under high-speed ball-milling, establishing an alkyl-anion-promoted polymerization process. However, the mechanism of the mechanochemical process differs from that of conventional anionic polymerizations, with mechanical force fracturing the newly formed polymer chains and generating macroradicals that participate in the polymerization process.
FARADAY DISCUSSIONS
(2023)
Article
Materials Science, Composites
Younghoon Kwon, Soyoung E. Seo, Jaejun Lee, Szabolcs Berezvai, Javier Read de Alaniz, Claus D. Eisenbach, Robert M. McMeeking, Craig J. Hawker, Megan T. Valentine
Summary: Additive manufacturing allows the creation of bio-inspired materials with complex architectures and diverse properties. By using a digital light processing strategy, polymer foams with controlled porosity were 3D printed by incorporating thermally expandable microspheres. The foams showed remarkable resilience under cyclic loading, maintaining their modulus and energy dissipation even at large deformations.
COMPOSITES COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Junhee Kim, Soonyoung Choi, Jinsu Baek, Yong Il Park, Jin Chul Kim, Ji-Eun Jeong, Hyocheol Jung, Tae-Hyuk Kwon, Byeong-Su Kim, Sang-Ho Lee
Summary: Topology control plays a critical role in determining the physical properties and potential applications of polymers, especially those with abundant hydrogen bonding donors and acceptors. This study focuses on poly(glycidoxy carbonyl benzoic acid)s (PGCs) and investigates the high-level control of inter- and intramolecular hydrogen bonding in topology-controlled PGCs. By introducing aromatic carboxylic acids into polyglycidols (PGs) through post-polymerization modification, three types of topology-controlled PGCs (linear, hyperbranched, and branched cyclic structures) were prepared. These PGCs showed pH-dependent self-association properties in solution and strong adhesive properties in the bulk state, with the branched cyclic PGC demonstrating a 2.6-fold enhanced adhesive property when mixed with topology-controlled PGs. This cooperative hydrogen bonding between polymer chains is expected to contribute to the development of advanced adhesives and have high potential in biological and biomedical applications due to its excellent biocompatibility.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Polymer Science
Sumin Lee, Woo Hyuk Jung, Minseong Kim, Dong June Ahn, Byeong-Su Kim
Summary: This study developed a method for the synthesis of degradable polyesters through the ring-opening alternating copolymerization of cyclic anhydrides and epoxides. The interplay between monomers was investigated, and the influence of monomer structure on the properties of the resulting polyesters was explored.
Article
Chemistry, Multidisciplinary
Robert D. Murphy, Colm Delaney, Srikanth Kolagatla, Larisa Florea, Craig J. Hawker, Andreas Heise
Summary: This study reports the design of photopolymerizable copolypeptides with tailored mechanical properties for additive manufacturing of 3D objects. The copolypeptides are able to form hydrogels suitable for direct ink writing or direct laser writing, leading to mechanically robust 3D structures.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Neha Choudhury, Ahyun Kim, Minseong Kim, Byeong-Su Kim
Summary: Poly(vinyl chloride) (PVC) is a widely used commodity plastic that is difficult to recycle and often discarded after use, causing environmental concerns. This study presents a mechanochemical degradation process that converts PVC into water-soluble biocompatible products. By introducing oxirane mechanophores into the polymer backbone and applying force, the polymer chain undergoes a ring-opening reaction, leading to the formation of acetals. Hydrolysis of the acetals further breaks down the polymer into low-molecular-weight fragments. This green alternative offers a solution to the environmental issues associated with PVC disposal.
ADVANCED MATERIALS
(2023)
Article
Polymer Science
Jiyoung Lee, Seonho Kim, Hyeoksu Kwon, Seungyun Jo, Du Yeol Ryu, U. Hyeok Choi, Byeong-Su Kim
Summary: Solid polymer electrolytes are potential alternatives to address safety concerns with liquid electrolytes. A new type of polyether-based single-ion-conducting solid polymer electrolyte was developed, which can be tailored with different functional groups. By introducing tri(ethylene glycol) and succinonitrile, the ionic conductivity of the electrolyte was significantly increased.
Article
Polymer Science
Yoichi Okayama, Taejun Eom, Michael Czuczola, Allison Abdilla, Jacob R. Blankenship, Kaitlin R. Albanese, Javier Read de Alaniz, Christopher M. Bates, Craig J. Hawker
Summary: The synthetic utility of heterotelechelic polydimethylsiloxane (PDMS) derivatives was enhanced by using a specifically designed silyl hydride (Si-H)-based initiator for anionic ring-opening polymerization (AROP) of hexamethylcyclotrisiloxane (D-3) monomers. The resulting PDMS polymers had high chain-end fidelity and heterotelechelic functionality. In situ termination of the propagating chain end with different chlorosilanes and functionalized alkenes further increased the diversity of the PDMS derivatives. The living nature of the polymerization allowed for the synthesis of narrow-dispersity polymers with a wide range of molar masses. Additionally, the feasibility of synthesizing supersoft bottlebrush networks using the PDMS macromonomers was demonstrated.
Article
Polymer Science
Gervase Ng, Zilong Wu, Tong Zhang, Anh Phong Dang, Yin Yao, Andrew R. J. Nelson, Stuart W. Prescott, Almar Postma, Graeme Moad, Craig J. Hawker, Cyrille Boyer
Summary: An oxygen-tolerant SI-PhotoRAFT technique has been developed for efficient synthesis of surface-tethered polymer brushes under low-energy near-infrared light. The technique takes advantage of the unique properties of NIR light to prepare polymeric coatings, even through barriers that are opaque to visible light. It enables precise modulation of brush height and sequential chain extension, as well as orthogonal control over polymerization and cross-linking processes using two different wavelengths.
Article
Multidisciplinary Sciences
Jihye Park, Ahyun Kim, Byeong-Su Kim
Summary: Despite recent advancements in mechanochemical polymerization, understanding the unique mechanochemical reactivity during the ball milling polymerization process still requires extensive investigations. Here, the authors use solid-state anionic ring-opening polymerization to synthesize polyethers from various functional epoxide monomers. The critical parameters of the monomers are investigated to elucidate the unique reactivity of ball milling polymerization. The controllable syntheses of the desired polyethers are characterized via NMR, GPC, and MALDI-ToF analyses. Interestingly, bulky monomers exhibit faster conversions in the solid-state in clear contrast to that observed for solution polymerization. Particularly, a close linear correlation is observed between the conversion of the ball milling polymerization and melting point of the functional epoxide monomers, indicating melting point as a critical predictor of mechanochemical polymerization reactivity.
NATURE COMMUNICATIONS
(2023)
Article
Polymer Science
Kaitlin R. Albanese, Jacob R. Blankenship, Timothy Quah, Amy Zhang, Kris T. Delaney, Glenn H. Fredrickson, Christopher M. Bates, Craig J. Hawker
Summary: The potential of ABC triblock terpolymers in improving the mechanical properties of thermoplastic elastomers is demonstrated by comparing them with symmetric ABA/CBC analogs having similar molecular weights and volume fraction of B and A/C domains. The ABC architecture enhances elasticity through full chain bridging between discrete hard domains, minimizing mechanically unproductive loops. In addition, ABC triblock terpolymers allow for a higher fraction of hard-block domains while maintaining elasticity, which is traditionally only possible with non-linear architectures or highly asymmetric ABA triblock copolymers. These advantages provide a tunable platform to create materials with practical applications while improving our fundamental understanding of chain conformation and structure-property relationships in block copolymers.
Article
Materials Science, Biomaterials
Gayoung Kwon, Jinsu Baek, Nuri Kim, Soonyoung Kwon, Nanhee Song, Seong-Cheol Park, Byeong-Su Kim, Dongwon Lee
Summary: By employing ultrastable polymeric micelles as drug carriers, the therapeutic efficacy and immunostimulating activity of oxidative stress amplifying hybrid prodrug (OSamp) could be fully maximized. Tumour-targeted OSamp-loaded micelles showed excellent colloidal stability and significant cytotoxicity to cancer cells, as well as induction of immunogenic cell death. In a syngeneic mouse tumour model, these micelles effectively inhibited tumour growth and activated adaptive immune responses, suggesting great translational potential as immunostimulating anticancer nanomedicine.
BIOMATERIALS SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Kihyuk Sung, Jinsu Baek, Soonyoung Choi, Byeong-Su Kim, Sang-Ho Lee, In-Hwan Lee, Hye-Young Jang
Summary: We have successfully synthesized a novel form of polyglycerol with an unprecedentedly low degree of branching (DB = 0.08-0.18), eliminating the need for glycidol protection. Leveraging the remarkable efficiency and selectivity of our Cu(triNHC) catalyst, we achieved a highly selective polymerization process. The ultralow-branched cyclic polyglycerol (DB = 0.08) synthesized at 0℃ showcased extraordinary characteristics, exhibiting the lowest diffusion coefficient and the highest molecular weight.
Review
Nanoscience & Nanotechnology
Yiqing Wang, Zhenzhen Wu, Faezeh Makhlooghi Azad, Yutong Zhu, Lianzhou Wang, Craig J. Hawker, Andrew K. Whittaker, Maria Forsyth, Cheng Zhang
Summary: The incorporation of fluorine into battery components can improve the energy density, safety, and cycling stability of rechargeable batteries. This review explores the design and utilization of fluorine-containing species in advanced batteries, examining the relationship between their chemical structure and battery performance. It also discusses the challenges and opportunities of fluorinated batteries within the present regulatory framework.
NATURE REVIEWS MATERIALS
(2023)