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The combined effect of matrix molecular weight, filler concentration, and filler-matrix interactions on the dynamic viscoelasticity of polydimethylsiloxane/clay composites

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Abstract

The macroscopic properties of particle-filled polymer melts depend sensitively on the state of particle dispersion and the structure and dynamics of the interfacial polymer layer, which, in turn, are governed by factors like polymer molecular weight (Mw), particle concentration (C), and particle-polymer interfacial interactions. However, the combined effect of these factors on the macroscopic properties is far from fully understood, especially for polymers filled with anisotropic particles. In this work, we investigate the combined effect of Mw, C, and polymer end-group (methyl, Me or hydroxyl, OH) on the dynamic viscoelastic behavior of polydimethylsiloxane (PDMS)/clay composites. The linear viscoelastic behavior of these composites follows a non-monotonic dependence on Mw, which varies considerably with a modification in C or the polymer end-group. Furthermore, for both Me-PDMS/clay and OH-PDMS/clay composites, the non-linear tests reveal either strain softening-hardening-softening or sustained softening beyond the linear regime, depending on the combination of C and Mw. The critical strains for the onset of softening and hardening vary differently with Mw for different combinations of C and the polymer end-group. Our results suggest that the morphology and rheological behavior of these composites are dictated by a complex interplay of various competing effects, namely, particle agglomeration, interfacial polymer packing and density, entanglements, and bridging interactions. These findings give insight into tailoring the properties of polymer composites by adjusting the combination of C, Mw, and particle-polymer interactions.

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The datasets used and/or analysed during the current study are available from the corresponding author on reasonable request.

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Acknowledgements

This work is supported by INSPIRE Faculty award (DST/INSPIRE/04/2014/001055), Department of Science and Technology, Government of India, and Early Career Research Award (ECR/2016/000228), Science and Engineering Research Board, Department of Science and Technology, Government of India.

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Correspondence to Asima Shaukat.

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Gavendra, A., Shaukat, A. The combined effect of matrix molecular weight, filler concentration, and filler-matrix interactions on the dynamic viscoelasticity of polydimethylsiloxane/clay composites. Rheol Acta 62, 641–663 (2023). https://doi.org/10.1007/s00397-023-01417-9

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  • DOI: https://doi.org/10.1007/s00397-023-01417-9

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