We report the first in-depth comparison of the mechanical properties and equilibrium solvent uptake of a range of polysiloxane nanocomposites based on treated and untreated montmorillonite and fumed silica nanofillers. We demonstrate the ability of equilibrium solvent uptake data (and, thus, overall physical and chemical cross-link density) to serve as a proxy for modulus (combining rubber elasticity and Flory-Rehner theory), hardness (via the theory of Boussinesq), and elongation at break, despite the nonideal nature of these networks. In contrast, we find that tensile and tear strength are not well-correlated with solvent uptake. Interfacial strength seems to dominate equilibrium solvent uptake and the mechanical properties it predicts. In the montmorillonite systems in particular, this results in the surprising consequence that equilibrium solvent uptake and mechanical properties are independent of dispersion state. We conclude that edge interactions play a more significant role than degree of exfoliation, a result unique in the field of polymer nanocomposites. This demonstrates that even a combination of polymer/nanofiller compatibility and thermodynamically stable nanofiller dispersion levels may not give rise to reinforcement. These findings provide an important caveat when attempting to connect structure and properties in polymer nanocomposites, and useful guidance in the design of optimized polymer/layered silicate nanocomposites in particular. © 2009 American Chemical Society.
Bibliographical noteKAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): KUS-C1-018-02
Acknowledgements: This work was supported by the Dow-Corning Corporation and the United States Office of Naval Research (ONR). Specific thanks go to Dr. Deborah Bergstrom and Dr. Timothy Chao for arranging for mechanical properties testing at Dow-Corning's Midland, MI facility, and to Jason Fisk, Kermit Kwan, and Dr. Carl Fairbank for performing the testing. EPG acknowledges the support of Award No. KUS-C1-018-02, made by King Abdullah University of Science and Technology (KAUST).
This publication acknowledges KAUST support, but has no KAUST affiliated authors.