Characterization and Modeling of Segmental Dynamics in Silicone Based Nanocomposites
The addition of nano-particles with novel chemical, optical, or barrier properties further opens the door to the development of so-called multifunctional materials (1). Key to developing robust, tailored composites is a detailed understanding of the structural contributions to the engineering properties of the composite and how they may change with time in harsh service conditions. The segmental dynamics and local order underlie much of the fundamental physics that influence the performance of elastomers and can serve as important diagnostics for reinforcement and other fundamental properties (e.g., network topology, cross-link density, the number and distance between chemical and physical (entanglements) cross-links, the type and volume fraction of filler) and thus provide a route to this fundamental understanding. {sup 1}H MQ-NMR spectroscopy has shown the ability to provide more reliable and quantitative information regarding the elastomer network structure and heterogeneities (2). {sup 1}H MQ-NMR methods allow for the measurement of absolute residual dipolar couplings (<{Omega}{sub d}>) and thus the segmental/cooperative dynamics Thus, the MQ-NMR method allows for the direct measure of network topology and in many cases, filler-particle interactions. The ability of MD methods to uncover structural motifs and dynamics at the atomistic scale is well known. In polymer systems, however, the relationship to bulk material properties can be somewhat tenuous due to often limited number of atoms and short time durations that can be studied. Extending these MD simulations to large assemblies of atoms and extending them to longer times using state of the art computational resources has allowed us to probe some useful relationships. MD provides static and dynamic properties for a collection of particles that allow atomic scale insights that are difficult to gain otherwise. We have been exploiting these methods to characterize the effects of network structure and filler content on a number of silicone based nanocomposite systems. This data is providing improved insight into the structural contributions to the changes in segmental dynamics. Here we provide an overview of our ongoing work toward understanding the influence of the network structure on the physical and chemical properties of advanced composite elastomers, including material performance in severe environments (high temperature, high strains, high radiation fluxes).
- Research Organization:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- W-7405-ENG-48
- OSTI ID:
- 964116
- Report Number(s):
- LLNL-PROC-412671; TRN: US200922%%109
- Resource Relation:
- Conference: Presented at: American Chemical Society Fall Meeting, Washington DC, DC, United States, Aug 16 - Aug 20, 2009
- Country of Publication:
- United States
- Language:
- English
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