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A rheological criterion to determine the percolation threshold in polymer nano-composites

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Abstract

In this work, the effect of multi-walled carbon nanotube (CNT) and montmorillonite nanoclay on polymer chain dynamics is investigated around the percolation concentration for systems based on ethylene vinyl acetate (EVA) copolymer. Then, the results obtained are compared with literature data to determine if, regardless of particle characteristics, a universal rheological behavior can be detected at percolation. To do so, rheological analyses are performed under small amplitude oscillatory shear (SAOS), large amplitude oscillatory shear (LAOS), and transient shear step. SAOS data showed that, while the dynamics related to the Rouse relaxation time (τ R) were not significantly influenced, the reptation relaxation time (τ D) was strongly increased by the presence of nanoparticles. In step shear transient tests, the critical shear rate \( \left({\dot{\upgamma}}_{\mathrm{cr}}\right) \) for overshoot appearance was decreased due to chain confinement, and the formation of particle network strongly increased the level of stress overshoot. Particle networks increased significantly the nonlinear parameters (I 3/I 1 and Q 0) obtained under LAOS and quantified by FT-rheology. In all measurements, due to the higher surface area associated to its size and density as well as hollow structure, CNT showed stronger effects compared to clay. Moreover, while the percolation concentration was different for CNT and clay, both systems showed similar behavior at percolation: a 0.5 scaling for G′ indicating a Rouse-dominated behavior.

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Acknowledgments

The authors acknowledge the financial support of Natural Sciences and Engineering Research Council (NSERC) of Canada and the Quebec Ministry for Economic Development, Innovation and Exportation (MDEIE) for this work. Financial support from the Arboranano center of excellence is also appreciated. Special thanks go to Southern Clay Products Inc. for nanoclay samples and CNano for carbon nanotube samples. Also, many thanks go to the group of Prof. Manfred Wilhelm at Karlsruhe institute of technology (KIT) during a student exchange period sponsored by Fonds Québécois de la Recherche sur la Nature et les Technologies (FQRNT).

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Authors and Affiliations

  1. Department of Chemical Engineering and CERMA, Université Laval, 1065 Avenue de la Médecine, Quebec, G1V 0A6, Canada

    Hojjat Mahi Hassanabadi & Denis Rodrigue

  2. Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology (KIT), Engesserstrasse 18, 76131, Karlsruhe, Germany

    Manfred Wilhelm

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  1. Hojjat Mahi Hassanabadi
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Correspondence to Denis Rodrigue.

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Hassanabadi, H.M., Wilhelm, M. & Rodrigue, D. A rheological criterion to determine the percolation threshold in polymer nano-composites. Rheol Acta 53, 869–882 (2014). https://doi.org/10.1007/s00397-014-0804-0

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