Mechanochemically responsive (MCR) polymers have been synthesized by incorporating mechanophores – molecules whose chemical reactions are triggered by mechanical force – into conventional polymer networks. Deformation of the MCR polymers applies force on the mechanophores and triggers their reactions, which manifest as phenomena such as changing colors, varying fluorescence and releasing molecules. While the activation of most existing MCR polymers requires irreversible plastic deformation or fracture of the polymers, we covalently coupled mechanophores into the backbone chains of elastomer networks, achieving MCR elastomers that can be repeatedly activated over multiple cycles of large and reversible deformations. This paper reports a microphysical model of MCR elastomers, which quantitatively captures the interplay between the macroscopic deformation of the MCR elastomers and the reversible activation of mechanophores on polymer chains with non-uniform lengths. Our model consistently predicts both the stress–strain behaviors and the color or fluorescence variation of the MCR elastomers under large deformations. We quantitatively explain that MCR elastomers with time-independent stress–strain behaviors can give time-dependent variation of color or fluorescence due to the kinetics of mechanophore activation and that MCR elastomers with different chain-length distributions can exhibit similar stress–strain behaviors but very different colors or fluorescence. Implementing the model into ABAQUS subroutine further demonstrates our model's capability in guiding the design of MCR elastomeric devices for applications such as large-strain imaging and color and fluorescence displays.
Journal of the Mechanics and Physics of Solids – Elsevier
Published: Sep 1, 2015
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