Hydrogen Bonding-Derived Healable Polyacrylate Elastomers via On-demand Copolymerization of n-Butyl Acrylate and tert-Butyl Acrylate

Achieving a desirable combination of good mechanical properties and healing efficiency is a great challenge in the development of self-healing elastomers. Herein, a class of tough and strong self-healing polyacrylate elastomers (denoted as HPs) was developed simply by free-radical copolymerization of n-butyl acrylate (nBA) and tert-butyl acrylate (tBA) and a subsequent hydrolysis reaction rather than direct copolymerization of nBA and acrylic acid (AA). The tiny difference in reactivity between nBA and tBA makes the structural units of the copolymer easy to control. Precise regulation of molecular composition can be realized just by varying the relative monomer content, making its mechanical properties to vary from ductile to robust. Strikingly, when HP samples are cut off within the gauge length, they can heal into coherent and smooth samples and recover at least 79% of the original strength. Hydrogen bond interactions serve as physical cross-linking points, contributing to the high mechanical performance (fracture energy of up to 73.78 MJ·m–3 and tensile strength of up to 17.80 MPa) as well as shape memory function. Moreover, the HP samples emit strong fluorescence when exposed to a 365 nm UV lamp and exhibit an aggregation-enhanced emission effect in the state of dissolution.