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Towards a rheological classification of flow induced crystallization experiments of polymer melts

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Abstract

Departing from molecular based rheology and rubber theory, four different flow regimes are identified associated to (1) the equilibrium configuration of the chains, (2) orientation of the contour path, (3) stretching of the contour path, and (4) rotational isomerization and a deviation from the Gaussian configuration of the polymer chain under strong stretching conditions. The influence of the ordering of the polymer chains on the enhanced point nucleation, from which spherulites grow, and on fibrous nucleation, from which the shish-kebab structure develops, is discussed in terms of kinetic and thermodynamic processes. The transitions between the different flow regimes, and the associated physical processes governing the flow induced crystallization process, are defined by Deborah numbers based on the reptation and stretching time of the chain, respectively, as well as a critical chain stretch. An evaluation of flow induced crystallization experiments reported in the literature performed in shear, uniaxial and planar elongational flows quantitatively illustrates that the transition from an enhanced nucleation rate of spherulites towards the development of the shish-kebab structure correlates with the transition from the orientation of the chain segments to the rotational isomerization of the high molecular weight chains in the melt. For one particular case this correlation is quantified by coupling the wide angle X-ray diffraction and birefringence measurements of the crystallization process to numerical simulations of the chain stretch of the high molecular weight chains using the extended Pom-Pom model in a cross-slot flow.

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Acknowledgement

The authors thank Frank Swartjes for providing the simulation results and experimental data for Figs. 3 and 4, Juan Vega for the discussion on the determination of τe for iPP, Ray Somani and Ben Hsiao for providing the molecular weight distribution of the melt in Somani et al. (2000, 2001) and Hans Christian Öttinger for critically reading the manuscript.

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Authors and Affiliations

  1. Institute of Polymers, Department of Materials, ETH, CH-8092, Zürich, Switzerland

    Jan van Meerveld

  2. Dutch Polymer Institute (DPI), Section Material Technology (MaTe), University of Technology Eindhoven, Eindhoven, The Netherlands

    Gerrit W. M. Peters

  3. Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA

    Markus Hütter

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van Meerveld, J., Peters, G.W.M. & Hütter, M. Towards a rheological classification of flow induced crystallization experiments of polymer melts. Rheol Acta 44, 119–134 (2004). https://doi.org/10.1007/s00397-004-0382-7

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