Jingkai Wang, Jie Sun, Jie Chen, Biao Kang, Ai Lu, Ruolei Zhong, Hongtu He, Guocheng Li, Chengji Wen, Dengtao Yang, Ying Yin
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Self-Assembled Entanglements in Elastomers for Superior Toughness and Fatigue Resistance
To address the long-standing trade-off between modulus, toughness, and fatigue resistance in elastomers, in this study, we propose an innovative strategy based on self-assembled chain entanglements. Unlike conventional strategies, the proposed entanglement-driven composite combines rigid, self-assembled entangled particles with a soft matrix enabled by strong interfacial adhesion. This system synergizes rigid entangled particles (with molecular segment entanglement topology) and the soft matrix to enable energy dissipation across molecular segments, polymer chains, and rigid entangled particles, ultimately achieving simultaneous enhancement of fracture toughness (∼0.043 MJ/m2), fatigue threshold (∼300 J/m2), and elastic modulus. Implemented via a one-step in situ self-assembly method, this strategy provides novel insights into designing high-performance elastomers.
期刊介绍:
Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.