The pursuit for functional nanocomposites that impact a wide range of technologies, ranging from information processing to energy storage / transducing devices has resulted in significant interest in the preparation of hybrid materials combining nanoparticles (NPs) with polymers. Current effort has specifically worked to achieve spatial-ordering of the NPs within structured polymer matrices. Ex-situ synthesis of NPs with tailored surface chemistry can be used for selective doping into chemically distinct regions of the polymer. Yet higher NP densities, inhibition of irreversible particle aggregation, and greater control in spatial distribution are accomplished by in-situ NP synthesis. Opportunities exist for developing facile, robust strategies for the In-situ synthesis of NPs in concert with the preparation of structured materials. To this end, we have explored adapting the principles of cascade synthesis for the production of single and two component NP composites. Specifically, we show that hierarchically structured NP network polymer composites can be prepared in a single “pot” through design of the molecular constituents which act to organize the reactive constituents (i.e., monomer, catalyst) to achieve multiple sequential or tandem reaction steps. Two systems will be presented. The first system employs a non-covalent, lamellar lyotropic mesophase composed of a supporting lipid matrix containing hydroxyl-and acrylate-end-derivatized triblock copolymers and the metal ion precursor. The second system is based on <i>N,N</i> dialkylimidazolium ionic liquid monomers self-assembled in water to form a structured lyotropic mesophase organizing a macromer (PEGDA), catalyst and the metal salt. Both routes yield durable, self-supporting and solvent responsive NP polymer composites possessing well-organized plasmonic Au NPs. Optical spectroscopy and TEM monitored the reduction of metal ions and evolution into nanoparticles. ATR/FT-IR spectroscopy and thermal analysis confirms acrylate crosslinking to yield the polymer network. X-ray scattering (SAXS and WAXS) monitored the evolution of the multi-lamellar structured mesophase and revealed the presence of semi-crystalline PEO confined within the water layers. Preliminary work demonstrating routes for the co-integration of emissive and plasmonic NPs will also be discussed.

Cascade synthesis of nanoparticle-polymer composites

253rd National Meeting (2017)

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