Polysiloxanes and Graphene: Two very different, yet uniquely versatile families of materials which, when combined can be utilized to design a vast range of complex and hierarchal 3-dimensional, flexible network architectures. At LLNL we have been making extensive use of these diverse and fascinating materials to design and synthesize some truly novel composites - with the potential for applications ranging from; flexible ultra-low ‘k’ dielectric coatings, negative temperature coefficient electronic switching materials, ultra-capacitors, electro-active materials, highly thermally resistant ablative materials and patterned media capable of large-scale isotropic dimensional change. Here we present a review of some of our recent efforts in this exciting and technologically relevant area of advanced materials science. The results of the synthesis and characterization (via a range of analytical methodologies including solid state NMR, degradative thermal analysis and broadband dielectric spectroscopy) of unique polysiloxane/carbon aerogel/carbon nanotube & graphene architectures will be presented. We will also present an overview of our ‘materials by design’ approach for the formation of 3-dimensional composite structures of sub-micron pattern resolution which can be triggered to undergo large-scale (fully reversible) isotropic changes in volume in response to external stimuli. Emphasis will be given to the relationship between the underlying (dynamic) network structure and the macro-scale physical properties of complex polysiloxane composites. And to the importance of combining a range of interrogative analytical methodologies with a ground up synthetic approach, in order to build well-defined & well understood materials at all size scales. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

Novel hierarchical composites of inorganic carbon and polysiloxanes for next-generation energy applications

249th National Meeting (2015)

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