Taking advantage of both the unique material properties of stimuli-responsive polymers with the design freedom enabled by additive manufacturing, has led to the rapid development of a variety of sophisticated functional materials. Often these materials have relied on chemical, light, or thermal stimuli to induce a response. To expand the scope of stimuli-responsive materials, the nascent field of polymer mechanochemistry looks to understand how force can be used as a productive stimulus to induce chemical changes. Polymer mechanochemistry has already proven a useful tool both in the preparation of stimuli-responsive materials, as well as to understand how mechanical force is transduced to the molecular level. Little work has been done, however, to understand how inherent stresses derived from polymer microstructure in phase-separated block-copolymers impacts the ability to activate mechanochemically active species within bulk polymer systems, and how this might be leveraged to create new stimuli-responsive and 3D-printed materials. To address this, we synthesized a series of block-copolymers with well-studied microphase separation behaviors that include an anthracene-maleimide mechanophore at the block-copolymer junction. We investigate both the bulk polymers and the ability to additively manufacture these materials, as well as interrogate the differences in the efficacy of the mechanochemically activated retro Diels-Alder reaction resulting from applied force to these systems.

Mechanochemical activation and additive-manufacturing of microphase-separating block-copolymer mechanophores

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ACS Fall 2022

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