Abstract
We correlate the terminal relaxation of supramolecular polymer networks, based on unentangled telechelic poly(isobutylene) linear chains forming micellar end-group clusters, with the microscopic chain dynamics as probed by proton NMR. For a series of samples with increasing molecular weight, we find a quantitative agreement between the terminal relaxation times and their activation energies provided by rheology and NMR. This finding corroborates the validity of the transient-network model and the special case of the sticky Rouse model, and dismisses more dedicated approaches treating the terminal relaxation in terms of micellar rearrangements. Also, we confirm previous results showing reduction of the activation energy of supramolecular dissociation with increasing molecular weight and explain this trend with an increasing elastic penalty, as corroborated by small angle x-ray scattering data.
Highlights
Supramolecular polymer networks with reversible crosslinking sites constitute a relatively new class of smart materials that are susceptible to various external stimuli to perform desired tasks such as self-healing and shape memory [1,2,3,4]
We correlate the terminal relaxation of supramolecular polymer networks, based on unentangled telechelic poly(isobutylene) linear chains forming micellar end-group clusters, with the microscopic chain dynamics as probed by proton NMR
For a series of samples with increasing molecular weight, we find a quantitative agreement between the terminal relaxation times and their activation energies provided by rheology and NMR
Summary
Supramolecular polymer networks with reversible crosslinking sites constitute a relatively new class of smart materials that are susceptible to various external stimuli to perform desired tasks such as self-healing and shape memory [1,2,3,4]. Terminal Flow of Cluster-Forming Supramolecular Polymer Networks: Single-Chain Relaxation or Micelle Reorganization? We correlate the terminal relaxation of supramolecular polymer networks, based on unentangled telechelic poly(isobutylene) linear chains forming micellar end-group clusters, with the microscopic chain dynamics as probed by proton NMR.
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