Journal
MACROMOLECULAR RAPID COMMUNICATIONS
Volume 42, Issue 1, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/marc.202000359
Keywords
coumarin; mechanochromism; nanocomposite; sonication
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Funding
- Michelin Americas Research and Development Corporation
- NSF [CHE-1808518, DMR-1121107]
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Molecular force probes, such as mechanochromophores, are useful tools for identifying vulnerable molecular sites under mechanical stress. A coumarin dimer mechanophore with strength similar to sulfur-sulfur bonds in vulcanized rubbers has been developed, allowing for detection of strain-induced scission within a polymer matrix. This study suggests that coumarin dimers serve as weak links within the matrix, similar to sulfur bridges in vulcanized rubbers.
Molecular force probes that generate optical responses to critical levels of mechanical stress (mechanochromophores) are increasingly attractive tools for identifying molecular sites that are most prone to failure. Here, a coumarin dimer mechanophore whose mechanical strength is comparable to that of the sulfur-sulfur bonds found in vulcanized rubbers is reported. It is further shown that the strain-induced scission of the coumarin dimer within the matrix of a particle-reinforced polybutadiene-based co-polymer can be detected and quantified by fluorescence spectroscopy, when cylinders of the nanocomposite are subjected to unconstrained uniaxial stress. The extent of the scission suggests that the coumarin dimers are molecular weak links within the matrix, and, by analogy, sulfur bridges are likely to be the same in vulcanized rubbers. The mechanophore is embedded in polymer main chains, grafting agent, and cross-linker positions in a polymer composite in order to generate experimental data to understand how macroscopic mechanical stress is transferred at the molecular scale especially in highly entangled cross-linked polymer nanocomposite. Finally, the extent of activation is enhanced by approximately an order of magnitude by changing the regiochemistry and stereochemistry of the coumarin dimer and embedding the mechanophore at the heterointerface of the particle-reinforced elastomer.
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