Elastomers with excellent and controllable mechanical properties have attracted tremendous interest and are the key to the development of advanced technologies. So far, a few promising methods, including addition of nanofillers and incorporation of physical interactions, have been developed to improve the performance. However, these previously reported approaches always fall into the modulus-extensibility trade-off with one increased while sacrificing the other. Here, we demonstrated that Young’s modulus and extensibility can be simultaneously enhanced by introducing rationally arranged ureidopyrimidone (UPy) units which possess strong quadruple H-bond interactions, leading to significantly improved toughness. Furthermore, by tuning the distribution of UPy units along the polymer chains, it was found that the formation of UPy clusters within the elastomers as well as the resulted Young’s modulus can be effectively modulated without affecting the elongation of the elastomers, which shows great advantage over conventional means of just changing the UPy concentrations. Finally, we proposed the dynamic processes taking place in the elastomers during stretching supported with clear experimental evidences. Our findings here lead to a deeper understanding on UPy-containing materials and will potentially be served as guidelines towards the design of next-generation high-performance elastomers.

Surpass the modulus- extensibility trade-off of elastomers by controlling the topology of physical interactions

ACS Spring Meeting 2021

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