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Traditional covalently cross-linked solid-state electrolytes exhibit desirable mechanical durability but suffer from limited processability and recyclability due to their permanent network structures. Incorporating dynamic covalent bonds offers a promising solution to these challenges. In this study, we report a reprocessable and recyclable polymer electrolyte based on a dynamic ester bond network, synthesized from commercially available materials. Polyethylene glycol diglycidyl ether (PEGDE) and glutaric anhydride (GA) were cross-linked and cured in the presence of benzyl dimethylamine (BDMA), forming an ester-rich polymer backbone. Subsequently, 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) was introduced as a transesterification catalyst to facilitate network rearrangement. Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was incorporated to establish efficient ion transport pathways. By tuning the cross-linking density and catalyst ratio, the electrolyte achieved an ionic conductivity of 1.89 × 10 S/cm at room temperature along with excellent reprocessability.
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http://dx.doi.org/10.3390/polym17141991 | DOI Listing |
Angew Chem Int Ed Engl
September 2025
Department of Chemistry, Colorado State University, Fort Collins, CO 80523, USA.
Adhesives are important in creating multilayer products, such as in packaging and construction. Most current hot-melt adhesives such as poly(ethylene-co-vinyl acetate) (EVA) and polyurethanes lack chemical recyclability and do not easily de-bond, complicating recycling. Here, we achieved tunable adhesive properties of chemically recyclable polyolefin-like multiblock copolymers through regulating the incorporation of crystalline hard blocks, amorphous soft blocks, and ester content highlighted by adhesive strengths up to 6.
View Article and Find Full Text PDFInt J Biol Macromol
September 2025
Key Lab of Rubber-Plastics, Ministry of Education/Shandong Provincial Key, Lab of Rubber-Plastics, School of Polymer Science and Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China. Electronic address:
A dynamically crosslinked network VEC (vulcanized ESO and CA) was synthesized in situ via zinc acetate-catalyzed epoxy ring-opening between epoxidized soybean oil (ESO) and anhydrous citric acid (CA), then incorporated into polylactic acid (PLA)/polybutylene adipate terephthalate (PBAT) blends to enhance interfacial compatibility. The dynamic ester-exchange network acted as an intermediate phase, improving the integration of the flexible PBAT phase within the rigid PLA matrix. VEC content critically influenced mechanical properties, with in-situ crosslinking during dynamic vulcanization enhancing chain interactions and blend homogeneity.
View Article and Find Full Text PDFChem Sci
August 2025
College of Polymer Science and Engineering, State Key Laboratory of Advanced Polymer Materials, Sichuan University Chengdu 610065 China
Polyphenol-derived vitrimers offer compelling prospects for sustainable materials owing to their intrinsic recyclability, reprocessability and biodegradability. However, practical development remains constrained by structure degradation under harsh reprocessing conditions and the need for sophisticated modifications of the bio-sourced precursors. Herein, we reported a strategy that integrates commercially available polyphenols and low-molecular-weight PDMS through adaptable iminoboronate chemistry, obviating the need for structural modifications.
View Article and Find Full Text PDFSmall
September 2025
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Reconciliation of the elasticity, reinforcement, and recyclability in elastomer nanocomposites (ENCs) remains challenging, primarily due to the energy losses of the friction at polymer-nanoparticle interfaces and the permanent covalent cross-linking. Here, a self-adaptive soft interface strategy is introduced, using modulus-tuned polymer nanoparticles (PNPs) as reinforcement agents and interfacial chemical cross-linking sites within a vitrimer elastomer matrix. Such a framework promotes synergistic deformation of the PNPs with the matrix chains during mechanical deformation to minimize energy dissipation.
View Article and Find Full Text PDFMacromol Rapid Commun
September 2025
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Institute of Science Tokyo, Meguro-ku, Tokyo, Japan.
Conventional cross-linked polymers are not recyclable or reprocessable due to the formation of permanent cross-links. Covalent adaptable networks (CANs) based on dynamic covalent chemistry attract great attention as materials that exhibit excellent stress relaxation, recyclability, reprocessability, and self-healing properties. Controlling the dynamic properties of CANs is important for both fundamental science and practical applications.
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