The ability to self-repair and resume active function upon incurring structural damage is an attribute of living organisms that has inspired research to enhance material performance and sustainability. Concepts that have been proven successful to instigate 'self-heal ability' comprise the integration of vessel-type reservoirs into materials, the integration of nanofillers to enable coupling to external fields, and the use of dynamic and reversible bond networks. While each of these concepts has shown promise, they are limited by manufacturing constraints, scalability, or cost and chemical sensitivity. An intriguing new concept for realizing self-repair capability in engineering polymers is based on copolymers with ‘interlocking chain architectures’.<br/><br/>This contribution will present recent progress in the understanding of the effect of copolymer brush architecture on the recovery behavior of brush particle-based hybrid materials. First, the methodology of using atom transfer radical polymerization to realize butyl acrylate (BA)/methyl methacrylate (MMA)-based copolymers with statistical, gradient and alternating architecture will be discussed. The effect of chain architecture on the microstructure and mechanical recovery behavior of linear and brush P(BA-co-MMA) copolymers will be presented. Tethering of chains to a surface will be shown to induce inhomogeneous microstructures with profoundly altered mechanical properties. Strategies to harness inhomogeneity formation to realize high modulus self-healing materials will be discussed.

Polymer design for accelerated recovery in brush-particle hybrid materials

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