Influence of molecular structure on rheological properties of polyethylenes |
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Authors: | H Münstedt Stefan Kurzbeck Lothar Egersdörfer |
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Institution: | (1) Institute of Polymer Materials Department of Materials Science University of Erlangen-Nürnberg Martensstr. 7 D-91058 Erlangen, Germany, DE |
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Abstract: | Elastic properties of melts of a long-chain branched low density polyethylene (LDPE) with a broad molecular mass distribution
and a short-chain branched linear low-density polyethylene (LLDPE) with a more narrow molecular mass distribution were investigated
by creep recovery measurements in shear. The results obtained by means of a magnetic bearing torsional creep apparatus in
the linear-viscoelastic region, showed that the steady state recoverable compliance of the LLDPE is greater by a factor of
two than that of the LDPE. In the short-time region up to 1000 s, however, the time-dependent recoverable compliance of the
LDPE is higher than that of the LLDPE. The retardation times for the LLDPE are considerably longer than for the LDPE. For
the LDPE the temperature dependence of the entanglement transition is consistent with that of the terminal zone of the creep
compliance. The activation energy of 58 kJ/mole lies in the typical range for long-chain branched polyethylenes. In the case
of the LLDPE the creep compliances can be shifted to give a mastercurve with an activation energy of 34 kJ/mole, whereas the
recoverable compliances do not follow the time-temperature superposition principle. The molecular characterization using TREF
showed that the LLDPE has a bimodal branching structure. In addition to a short-chain branched component, a low percentage
of a linear constituent with high molecular mass was found. It is postulated that this linear component forms a dispersed
phase in the matrix of the short-chain branched constituent. The resulting interfacial tension could be the reason for the
long retardation times, the high steady state recoverable compliance and the fact that the time-temperature superposition
principle is not fulfilled in the case of the LLDPE investigated.
Received: 1 July 1997 Accepted: 12 November 1997 |
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Keywords: | LDPE- and LLDPE-melts creep recovery retardation spectra branching distribution interfacial tensions |
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