From Slow to Fast Self-Healing at Ambient Temperature of High-Modulus Reversible Poly(methacrylate) Networks. Single- and Dual-Dynamics and the Effect of Phase-Separation.

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Abstract

Reversible poly(methacrylate) networks are synthesized with tunable thermomechanical and self-healing properties. The focus is on high-modulus networks (guide value around 500 MPa at 25 °C) in combination with fast self-healing for applications as coatings at ambient temperature. In case of a broad temperature window for outdoor applications, mechanical robustness up to 120 °C is aimed for. Methacrylate-functionalized Diels-Alder prepolymers containing furan-maleimide reversible covalent bonds are first synthesized at 25 °C. The prepolymers act as reversible crosslinkers in the subsequent UV-polymerization at 60 °C. Reaction-induced phase-separation is achieved by changing the balance between soft and hard blocks, leading to homogeneous and (partially) phase-separated, fully reversible poly(methacrylate) networks. The incorporation of urethane bonds introduces hydrogen bonding capacity. For comparison, irreversible poly(methacrylate) networks, i.e. without reversible Diels-Alder bonds, are synthesized via UV-polymerization of irreversible methacrylate-functionalized prepolymers. A tunable self-healing behavior is demonstrated. The single-dynamic high-modulus poly(methacrylate) networks, i.e. purely based on reversible Diels-Alder bonds, show slowest self-healing, e.g. 7 days in ambient conditions. The dual-dynamic high-modulus poly(methacrylate) networks, i.e. based on covalent Diels-Alder bonding and supramolecular hydrogen bonding, show fastest self-healing, e.g. 10 min in ambient conditions, if hydrogen bonding is combined with intrinsic local network mobility in case of a (partially) phase-separated network morphology.
Original languageEnglish
Pages (from-to)9960-9977
Number of pages18
JournalMacromolecules
Volume54
Issue number21
DOIs
Publication statusPublished - 9 Nov 2021

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