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Complex dynamics of hydrogen bonded self-assembling polymers

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5 Author(s)
M. Wubbenhorst ; Fac. of Appl. Sci., Delft Univ. of Technol., Netherlands ; J. van Turnhout ; B. J. B. Folmer ; R. P. Sijbesma
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Supramolecular polymers, which are non-covalently bonded and formed by self association of di or trifunctional monomers exhibit, by virtue of quadruple hydrogen bonds, many of the properties of normal high molecular weight polymers, e.g. a dynamic rubber plateau. We focus on the molecular and cooperative dynamics of self-assembled linear polymers and networks, studied by broadband dielectric relaxation spectroscopy (DRS) in the frequency range from 10-2 to 106 Hz. The DRS analysis was backed up by dynamic mechanical and rheological experiments. In the high temperature region two loss processes (α and α*) show up, the relaxation times of which obey the Vogel-Fulcher-Tammann (VFT) law. The dielectric α process is related to the dynamic glass-rubber transition and is slightly faster than the corresponding mechanical α process. A slower (high-temperature) α* relaxation is identified as chemical, corresponding to the mean lifetime of the hydrogen bonded linkages in the supramolecular chains. Its relaxation time τα* was found to be 1 to 2 decades larger than the terminal flow relaxation time, indicating that the relaxation of an entire chain is dominated by the joint dynamics of many hydrogen bonds. The β relaxation, observed in both DRS and dynamic mechanical analysis (DMA) at temperatures below Tg, arises from the local junction dynamics of hydrogen bonded units in the glassy state. Details of the temperature dependence and the shape of the loss peaks of the α and α* relaxations will be discussed in terms of temporary physical networks and cooperativity

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IEEE Transactions on Dielectrics and Electrical Insulation  (Volume:8 ,  Issue: 3 )