Journal
NATURE MATERIALS
Volume 21, Issue 1, Pages 103-+Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41563-021-01124-x
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Funding
- Leverhulme Trust Program Grant (Natural Materials Innovation)
- Marie Skodowska-Curie Fellowship [845640]
- Cambridge Display Technology (CDT)
- Engineering and Physical Sciences Research Council [EP/R512461/1]
- Marie Curie Actions (MSCA) [845640] Funding Source: Marie Curie Actions (MSCA)
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This study introduces non-covalent crosslinkers with slow dissociation kinetics, enabling the formation of glass-like supramolecular networks with high compressibility. These materials exhibit high compressive strengths and fast self-recovery, holding promise for high-performance soft materials in various applications such as soft robotics and tissue engineering.
Supramolecular polymer networks are non-covalently crosslinked soft materials that exhibit unique mechanical features such as self-healing, high toughness and stretchability. Previous studies have focused on optimizing such properties using fast-dissociative crosslinks (that is, for an aqueous system, dissociation rate constant k(d) > 10 s(-1)). Herein, we describe non-covalent crosslinkers with slow, tuneable dissociation kinetics (k(d) < 1 s(-1)) that enable high compressibility to supramolecular polymer networks. The resultant glass-like supramolecular networks have compressive strengths up to 100 MPa with no fracture, even when compressed at 93% strain over 12 cycles of compression and relaxation. Notably, these networks show a fast, room-temperature self-recovery (< 120 s), which may be useful for the design of high-performance soft materials. Retarding the dissociation kinetics of non-covalent crosslinks through structural control enables access of such glass-like supramolecular materials, holding substantial promise in applications including soft robotics, tissue engineering and wearable bioelectronics.
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