Journal of the American Chemical Society · 2018 · 165 citations · 55 references
Natural SciencesMaterials EngineeringMaterials ScienceMaterials ChemistryPolymer ChemistryPolymer MaterialsElastomeric PolymersIntermolecular ForcesStress-strain BehaviorFracture BehaviorMaterial Fracture BehaviorSilicone ElastomersSpiropyran CompoundsStress DistributionStress-strain RelationsStress-strain RelationshipsTensile Deformation Of Polymers
Mechanochromic force probes, such as spiropyran derivatives, enable visualization of stress/strain distribution and fracture behavior in polymeric materials. This study examines the macroscopic response of silicone elastomers cross‑linked with three spiropyran regioisomers. The spiropyran derivatives SP(o), SP(m), and SP(p) are incorporated into the network via the same attachment point on the indoline fragment, with regioisomeric attachments ortho, meta, and para to the spirocyclic C‑O bond on the benzaldehyde fragment. Under quasi‑static uniaxial tension, the colorimetric response follows SP(o) > SP(m) > SP(p), but all three exhibit indistinguishable strain onset at ~90% strain, and their ratiometric response remains constant across 90–135% strain, contrary to simulation predictions.
Mechanochromic force probes, including spiropyran derivatives, have proven to be useful in visualizing the stress/strain distribution and fracture behavior in polymeric materials. Here, we report the macroscopic response of silicone elastomers including cross-links made up of three spiropyran (SP) regioisomers. The SP derivatives SP( o), SP( m), and SP( p) are connected to the network through an identical attachment point on the indoline fragment and regioisomeric attachments ortho, meta, and para to the spirocyclic C-O bond on the benzaldehyde fragment, respectively. The relative colorimetric response of these regioisomers under quasi-static uniaxial tensile load is SP( o) > SP( m) > SP( p), consistent with the expected mechanical sensitivity of the regioisomers obtained from molecular modeling. The extrapolated strain onset for detectable activation of all three regioisomers, however, is indistinguishable and occurs at ∼90% uniaxial strain. Finally, the ratiometric response of the three isomers is constant across the strains investigated (90-135% uniaxial strain), in contrast to expectations based on simulations of strained intact polymer networks.
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