Abstract
The hardness of thermoplastic elastomers (TPEs) significantly influences their suitability for various applications, but traditionally, enhancing hardness reduces toughness. Herein a method is introduced that leverages hybrid soft segments to fine-tune the hardness of TPEs without compromising their exceptional toughness. Through the selective copolymerization of polytetramethylene ether glycols (PTMEGs) at various molecular weights, supramolecular poly(urethane-urea) TPEs are molecularly engineered to cover a wide spectrum of hardness while retaining good toughness. It is achieved through the formation of graded functional zones-densely packed for enhanced hardness and strength, and loosely packed for greater extensibility and toughness-driven by variations in PTMEG chain length and mismatched supramolecular interactions. Through the establishment and systematic investigation of a TPE library, the intricate interplay between design, structure, and performance of these materials is elucidated, refining the optimization techniques. The TPEs demonstrate exceptional mechanical properties, including a variant with a Shore hardness of 86A and a toughness of 819MJm-3, alongside a softer variant with a 59A hardness and a 786MJm-3 toughness. The innovation extends to a scalable solvent-based TPE production line, promising widespread industrial application. This advancement reimagines the potential of high-performance TPEs and composites, offering versatile materials for demanding applications.
Published Version
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