Article
Polymer Science
Alessandro Angelini, Anja Car, Ionel Adrian Dinu, Luigi Leva, Wilfredo Yave
Summary: Tailor-made poly(vinyl alcohol)-b-poly(styrene) copolymers (PVA-b-PS) for separation membranes are synthesized using reversible-deactivation radical polymerization techniques. These di-block copolymers have high molecular weight (>70 kDa), high PVA content (>80 wt%), and good film-forming property. They self-assemble in aqueous media to form micelles, which when cast on a porous substrate, result in thin-film membranes with higher water permeance than that of PVA homopolymer. The PS nanodomains within the PVA matrix act as cross-linking points, eliminating the need for chemical cross-linkers and acid catalysts. Thermal annealing further enhances membrane selectivity through improved microphase separation.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Jared I. Bowman, Cabell B. Eades, Maria A. Vratsanos, Nathan C. Gianneschi, Brent S. Sumerlin
Summary: Polymerization-induced self-assembly (PISA) is a powerful technique for producing block copolymer nanostructures, and ultrafast photoiniferter PISA can be used to quickly create various nanostructures.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Polymer Science
Chia-Juei Hsu, Cheng-Wei Tu, Yu-Wen Huang, Shiao-Wei Kuo, Rong-Ho Lee, Yu-Ting Liu, Han-Yu Hsueh, Junko Aimi, Chih-Feng Huang
Summary: In this study, poly (styrene)-b-poly (2-vinyl pyridine) four-arm star block copolymers with high interaction parameter feature were successfully synthesized, and their self-assembly behaviors in nanoscale including cylinder and lamellae morphologies were observed.
Article
Polymer Science
Lei Guo, Dingli Xia, Yaping Wang, Shipeng Ding, Junting Xu, Yutian Zhu, Binyang Du
Summary: This study employed a single surfactant CTAB and a series of symmetrical VmS24.2kVm triblock copolymers with different molecular weights of P4VP blocks to fabricate various complex-shaped particles via 3D-SCSA. The external shape and internal morphology of the particles were closely related to the volume fraction of the P4VP block and the concentration of CTAB.
Article
Polymer Science
Robert Mundil, Alexander Zhigunov, Mariusz Uchman
Summary: In this study, we synthesized and self-assembled mPEG-block-PDL-block-PMMA triblock terpolymers using a metal-free catalytic system, which showed better polymerization control compared to sequential copolymerization. The blocks were found to be incompatible, leading to their self-assembly into multicompartment micelles in water.
EUROPEAN POLYMER JOURNAL
(2022)
Review
Polymer Science
Lin-Lin Xiao, Xu Zhou, Kan Yue, Zi-Hao Guo
Summary: Conjugated block copolymers (cBCPs) are promising materials with high conductivity and morphological versatility, making the study of their self-assembly behaviors crucial for enhancing device performance.
Article
Biochemistry & Molecular Biology
Mariia Levit, Alena Vdovchenko, Apollinariia Dzhuzha, Natalia Zashikhina, Elena Katernyuk, Alexey Gostev, Eugene Sivtsov, Antonina Lavrentieva, Tatiana Tennikova, Evgenia Korzhikova-Vlakh
Summary: Novel bio-inspired amphiphilic block-copolymers were synthesized and self-assembled into nanoparticles of approximately 200 nm in aqueous media, demonstrating enhanced thermal stability, low cytotoxicity, and retained biological activity against lung adenocarcinoma epithelial cells.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Article
Chemistry, Physical
Voitto Kankanen, Micaela Fernandes, Zehua Liu, Jani Seitsonen, Sami-Pekka Hirvonen, Janne Ruokolainen, Joao F. Pinto, Jouni Hirvonen, Vimalkumar Balasubramanian, Helder A. Santos
Summary: This study reports the development of poly(ethylene glycol)-block-(e-caprolactone) (PEG-b-PCL) nanoparticles using a microfluidic technique for intravenous drug delivery. The optimized formulation achieved spherical morphology, small particle size (dH < 80 nm), uniform size distribution (PDI < 0.2), high drug loading degree (16%), and encapsulation efficiency of 54%. Furthermore, the nanoparticles exhibited stability and sustained release of sorafenib in vitro over several days. Overall, this research demonstrates the use of microfluidic approach in optimizing drug delivery systems.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Biochemistry & Molecular Biology
Elena Yu. Kozhunova, Anna V. Plutalova, Andrey V. Sybachin, Alexander V. Chertovich, Elena V. Chernikova
Summary: This study investigated the double stimuli-responsive properties of PNIPA and PVIM block copolymers in aqueous solutions for the first time. The synthesis of two different block copolymers was performed using RAFT polymerization. The conformational behavior and self-assembly ability of the polymers were found to depend on the location of hydrophobic groups derived from the RAFT agent within the chain, as well as the length and charge of the PVIM block.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Editorial Material
Nanoscience & Nanotechnology
Kevin G. Yager
Summary: The self-assembly of a triblock bottlebrush polymer at one length scale determines the organization of the self-assembly at a smaller scale, creating a hierarchical unit cell.
NATURE NANOTECHNOLOGY
(2023)
Article
Chemistry, Physical
Frank Hartmann, Martin Bitsch, Bart-Jan Niebuur, Marcus Koch, Tobias Kraus, Christian Dietz, Robert W. Stark, Christopher R. Everett, Peter Mueller-Buschbaum, Oliver Janka, Markus Gallei
Summary: This study synthesized a high-molecular-weight polystyrene-b-poly(methyl methacrylate) block copolymer as a soft matrix to fabricate nanocomposites containing magnetic nanoparticles. The influence of different ratios of PMMA-coated FePt nanoparticles on the self-assembled morphology was investigated. Statistical analysis revealed that the particles mainly self-assembled inside the PMMA phase at low particle concentrations, while higher particle ratios had a negative effect on the morphology. The magnetic addressability of the nanoparticles inside the nanocomposite films was confirmed using bimodal magnetic force microscopy.
Article
Environmental Sciences
Ming Hang Tai, Babu Cadiam Mohan, Zhiyi Yao, Chi-Hwa Wang
Summary: The superhydrophobic composite aerogel prepared from industrial waste-derived leached carbon black waste and polyvinyl alcohol showed excellent oil-water separation performance and selective adsorption capabilities, making it an effective solution for the remediation of oil spills.
Article
Polymer Science
Inna O. Lebedeva, Ekaterina B. Zhulina, Oleg V. Borisov
Summary: Research indicates that block copolymers with chemically different bottlebrush blocks can self-assemble into nanostructures resembling micelles in selective solvents. The self-consistent field theoretical approach is utilized to predict the relationship between structural parameters of bottlebrush blocks and properties of micelles, including critical micelle concentration. Theoretical predictions suggest that replacing linear blocks with bottlebrush ones of the same polymerization degrees leads to changes in micellar core size and corona extension, as well as an increase in critical micelle concentration, which are in agreement with computer simulation results.
Article
Polymer Science
Hyeongkeon Yoon, Seonghyeon Ahn, Qingshu Dong, Chungryong Choi, Eunyoung Kim, Weihua Li, Jin Kon Kim
Summary: This study investigated the formation of a multidomain double-stranded helical nanostructure, paving the way for the creation of multifunctional helical structures for various applications such as metamaterials. The experimentally observed morphology matched well with the prediction by self-consistent field theory.
Article
Chemistry, Multidisciplinary
Yuwei Liu, Xiaona Cui, Yong-Ill Lee, Hong-Guo Liu
Summary: This study systematically investigated the self-assembly behavior of polystyrene-block-poly(2-vinylpyridine) at the liquid/liquid interface. Different primary morphologies of aggregates were obtained depending on the molecular structure of the block copolymers and the amount of chloroauric acid. The findings provide valuable insights into the self-assembly behavior of block copolymers at interfaces and offer a facile approach for fabricating functional structures.
Article
Chemistry, Physical
Xuetong Li, Alba Villar-Yanez, Charlene Ngassam Tounzoua, Jordi Benet-Buchholz, Bruno Grignard, Carles Bo, Christophe Detrembleur, Arjan W. Kleij
Summary: We have developed a silver-catalyzed cascade conversion method for the selective formation of keto-functionalized cyclic carbonates using modular alkyne-1,n-diols and carbon dioxide. This method is characterized by its operational simplicity, excellent scope of carbonate-based heterocycles, and mild reaction conditions.
Article
Polymer Science
Florent Monie, Bruno Grignard, Christophe Detrembleur
Summary: This study reports an approach to fabricate self-blown nonisocyanate polyurethane (NIPU) foams by utilizing the divergent chemistries of amines with cyclic carbonates, creating the polymer network and thiolactone, and delivering in situ a thiol that generates the blowing agent (CO2) by reaction with a cyclic carbonate. The foams can be easily repurposed into films or structural composites by thermal treatment, showing recyclability. This facile and robust process offers new possibilities for designing more sustainable PU foams and provides options for end-of-life repurposing.
Article
Chemistry, Physical
Antoine Brege, Bruno Grignard, Raphael Mereau, Christophe Detrembleur, Christine Jerome, Thierry Tassaing
Summary: This review examines the state-of-the-art routes for synthesizing CO2-based (a)cyclic carbonates and polycarbonates from alcohol substrates. The first section focuses on the synthesis of organic carbonates from alcohol carbonation, discussing different strategies and substrates used. The second section discusses the formation of polycarbonates through direct copolymerization of CO2 with diols, as well as the ring-opening polymerization route. Finally, the polycondensation processes involving CO2-based dimethyl and diphenyl carbonates with aliphatic and aromatic diols are described.
Review
Chemistry, Multidisciplinary
Charlene Ngassam Tounzoua, Bruno Grignard, Christophe Detrembleur
Summary: This Review summarizes the recent advances in the synthesis of exovinylene cyclic carbonates, which can be produced from renewable and inexhaustible carbon dioxide as an alternative to fossil resources. The article focuses on describing the catalysts needed for their preparation and discussing the unique reactivity of these CO2-based heterocycles for the construction of diverse organic building blocks and (functional) polymers. The challenges and the future perspectives in the field are also discussed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Fabiana Siragusa, Jeremy Demarteau, Thomas Habets, Ion Olazabal, Koen Robeyns, Gwilherm Evano, Raphael Mereau, Thierry Tassaing, Bruno Grignard, Haritz Sardon, Christophe Detrembleur
Summary: In this study, a new depolymerization method for step-growth polymers is reported, which can be degraded into their native precursor or added-value offspring, while generating hemiacetal cyclic carbonate. The specific functionalities in the polymer trigger degradation at a certain temperature and in the presence of an organic base catalyst, and can be fully degraded within 2 hours without the need for solution conditions.
Article
Chemistry, Multidisciplinary
Ashish Raj, Satyannarayana Panchireddy, Bruno Grignard, Christophe Detrembleur, Jean-Francois Gohy
Summary: A sustainable bio-based solid-state electrolyte was developed based on carbonated soybean oil, which exhibited good ion conductivity and electrochemical stability at both room temperature and high temperature, and showed promising performance in lithium batteries.
Article
Chemistry, Multidisciplinary
Fabiana Siragusa, Thomas Habets, Raphael Mereau, Gwilherm Evano, Bruno Grignard, Christophe Detrembleur
Summary: Designing easily degradable polymers is crucial to reduce the accumulation of post-consumer plastic waste. In this study, regioregular polycarbonates prepared by organocatalyzed copolymerization were chemically recycled, providing a feasible method for the synthesis of novel degradable polymers.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Maxime Bourguignon, Bruno Grignard, Christophe Detrembleur
Summary: This article reports a simple and scalable process for preparing non-isocyanate polyurethane (NIPU) foams. The process replaces the previous use of toxic isocyanate-based chemistry with a more sustainable variant that forms CO2 through the hydrolysis of a comonomer. The process allows for the production of greener polyurethane foams using readily available low-cost starting materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biochemistry & Molecular Biology
Anna Pierrard, Abdelhafid Aqil, Christophe Detrembleur, Christine Jerome
Summary: This study investigates isocyanate-free formulations for poly(propylene glycol) polyurethane elastomers and examines two curing approaches. The results show that both methods provide highly cross-linked polymer networks with excellent mechanical properties. The developed UV-activated formulation is suitable for 3D printing.
Article
Chemistry, Multidisciplinary
Manuel Cardosa-Gutierrez, Guillaume De Bo, Anne-Sophie Duwez, Francoise Remacle
Summary: Substituted furan-maleimide Diels-Alder adducts connected by dynamic covalent bonds exhibit high attractiveness in mechanophores. Thermally activated [4 + 2] retro-Diels-Alder (DA) reactions proceed mainly through a concerted mechanism. An asymmetric mechanical force along the anchoring bonds in proximal dimethyl furan-maleimide adducts favors a sequential pathway. The findings provide a basis for the rational design of DA mechanophores in polymer science and photochemistry.
Article
Chemistry, Multidisciplinary
Matteo Calvaresi, Anne-Sophie Duwez, David A. Leigh, Damien Sluysmans, Yiwei Song, Francesco Zerbetto, Liang Zhang
Summary: The mechanical response of synthetic small-molecule trefoil knots, including their relative rigidity, higher resistance to external loads compared to biological knots, fast recovery of conformation after mechanical perturbation, and the importance of tightening in accommodating mechanical stress, is investigated through single-molecule pulling experiments.
Article
Materials Science, Multidisciplinary
Alvaro Gomez-Lopez, Bruno Grignard, Inigo Calvo, Christophe Detrembleur, Haritz Sardon
Summary: By combining NH2-PHU-NH2, epoxy resin, and thiol compound, high-shear strength PHU-epoxy hybrid adhesives can be developed and cured at room temperature in short times. These adhesives exhibit superior toughness without compromising lap-shear strength and shear resistance under load and temperature, making them suitable for high-demand applications in the automotive industry.
ACS APPLIED POLYMER MATERIALS
(2022)
Article
Polymer Science
Rayna Bryaskova, Nikoleta Philipova, Nikolai Georgiev, Damyan Ganchev, Ivo Lalov, Christoph Detrembleur
Summary: Novel bio-inspired photoactive antibacterial polymer coatings were prepared on stainless steel, exhibiting good mechanical and antibacterial properties. The coatings consisted of three components deposited on the stainless steel substrate: a catechol-based cationic glue as a universal primer, a silver-loaded nanogel decorated with o-quinones to enhance antibacterial properties and permit photosensitizer grafting, and an ethylene diamine derivative of protoporphyrin IX. The antibacterial activity of the coatings was confirmed against both Gram-positive and Gram-negative strains, making them promising for medical and biomedical applications.
JOURNAL OF POLYMER RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Fabiana Siragusa, Thomas Habets, Raphael Mereau, Gwilherm Evano, Bruno Grignard, Christophe Detrembleur
Summary: This study presents a new type of degradable polymer that can be easily and completely degraded into its monomers under mild conditions through catalyst-free aminolysis. The recovered monomers can then be used for polymer synthesis, offering a closed-loop recycling scenario. This work is of great significance for addressing the accumulation of post-consumer plastic waste and providing building blocks for the synthesis of novel degradable polymers.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Polymer Science
Thomas Habets, Fabiana Siragusa, Alejandro J. Mueller, Quentin Grossman, Davide Ruffoni, Bruno Grignard, Christophe Detrembleur
Summary: This study presents a facile and efficient method for constructing copolymers containing both oxazolidone and thiocarbonate linkages. The one-pot terpolymerization process can be conducted at room temperature without the need for catalysts. The resulting copolymers have high solubility and can be used as adhesives. Additionally, a simple thermal treatment can achieve quantitative dehydration and the pendant double bonds allow for facile thiol-ene functionalization.