Journal
ADVANCED MATERIALS
Volume 33, Issue 23, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202008523
Keywords
elastomers; fracture toughness; octuple hydrogen bonding; stiffness; toughening mechanisms
Categories
Funding
- Research Council of Norway [255507, 245963]
- JSPS KAKENHI [JP18H03753, JP18K18807, JP18H05241]
- Ministry of Education, Youths and Sports of the Czech Republic within the project CEITEC 2020 [LQ1601]
- National Natural Science Foundation of China [11772278]
- Jiangxi Provincial Outstanding Young Talents Program [20192BCBL23029]
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A transparent unfilled elastomer with enhanced toughness and stiffness is achieved by incorporating ultrastrong, reversible, and sacrificial octuple hydrogen bonding (HB). The homogeneous network structure distributes stress evenly to each polymer chain, enhancing stretchability and delaying fracture. Strong HBs and corresponding nanodomains enhance stiffness by restricting network mobility, while simultaneously improving toughness by dissipating energy during configuration transformation.
Current synthetic elastomers suffer from the well-known trade-off between toughness and stiffness. By a combination of multiscale experiments and atomistic simulations, a transparent unfilled elastomer with simultaneously enhanced toughness and stiffness is demonstrated. The designed elastomer comprises homogeneous networks with ultrastrong, reversible, and sacrificial octuple hydrogen bonding (HB), which evenly distribute the stress to each polymer chain during loading, thus enhancing stretchability and delaying fracture. Strong HBs and corresponding nanodomains enhance the stiffness by restricting the network mobility, and at the same time improve the toughness by dissipating energy during the transformation between different configurations. In addition, the stiffness mismatch between the hard HB domain and the soft poly(dimethylsiloxane)-rich phase promotes crack deflection and branching, which can further dissipate energy and alleviate local stress. These cooperative mechanisms endow the elastomer with both high fracture toughness (17016 J m(-2)) and high Young's modulus (14.7 MPa), circumventing the trade-off between toughness and stiffness. This work is expected to impact many fields of engineering requiring elastomers with unprecedented mechanical performance.
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