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Title: The Role of Nanofillers in Polymer Nanocomposites
Authors: Gersappe, Dilip
Xu, Di
Department of Materials Science and Engineering
Rafailovich, Miriam
Sokolov, Jonathan
Grubbs, Robert B.
Issue Date: 1-Dec-2016
Publisher: The Graduate School, Stony Brook University: Stony Brook, NY.
Abstract: Polymer nanocomposites have been widely used in many fields. By introducing nanoparticles as fillers, researchers are able to get reinforced materials and new materials with novel properties, such as stronger mechanics, enhanced optical properties and improved conductivity. Though experimental techniques have rapidly advanced to enable better control of materials at atomic level, there is still a lack of a fundamental understanding of the dynamics and structure-properties relations in polymer nanocomposites. In this thesis, we use computer simulations to study the molecular structure and connections between microstate to macro properties of a variety of nanocomposites. Our goal is to understand the role of nanofillers in complex nanocomposite systems and to assist nanocomposite design. Nanoplatelet fillers, such as clays, have shown superior effects on the properties of polymer gels. We used molecular dynamic simulation to study nanoplatelet-filled composite gel system, in which short-range attraction exists between the polymer and nanoplatelet fillers. We show that the polymers and nanoplatelet fillers formed organic-inorganic networks with nanoplatelets acting as crosslink junctions, and the network eventually percolates the system as fillers reached a critical concentration. Stress auto-correlation and step-strain test were applied to investigate the mechanical properties; the results show the simulated composites changed from fluid-like to solid-like. The mechanical changes were consistent with the percolation transition, and gelation mechanism was therefore believed to be similar to those pure polymer physical gels. It was observed platelets aggregated into a local intercalation structure, which significantly differs from typical spherical fillers. This unique intercalation structure was examined by radial distribution function and ordering parameters. We discussed how intercalation would affect the properties of the platelet composites by comparing them with spherical fillers. Nanofillers have been widely used in polymer blends to improve the interfacial compatibility of otherwise immiscible polymers. In the second system, we investigated the interfacial behavior of binary polymer blends with different types of fillers. The interfacial tension and shear resistance were studied as a function of filler-polymer interaction, filler concentration and species of fillers. We found filler-polymer interaction is the key factor to improve the interfacial compatibility. The results show that nanofillers reduce both interfacial tension and interfacial slip at strong filler-polymer interaction. The effects of nanofillers however differ significantly from each other by their shapes. We analyzed the structure of nanofillers at the interface and their effects on the interfacial behaviors. The self-assembly of polymers into a columnar structure, while subject to a thin film environment, provides an economic route to fabricate polymer solar cell (PSC) with high conversion efficiency. In our work, we showed that two immiscible polymer segregates into to a percolating columnar structure when confined to a thin film. By adding nanofillers, with specific functionality, we can template the segregation of nanofillers to the polymer-polymer interface. We prove this process is surface tension driven and is a result that is particular for thin film geometries, where the thickness is under critical value. The results provide a theoretical basis for the column structure forming in a self-assembled PSC system, and can help to select polymer candidates that optimize PSC efficiency. These studies serve as theoretical guideline for engineering novel nanocomposites, and could lead to the design of materials with new and improved properties.
Description: 93 pg.
Appears in Collections:Stony Brook Theses and Dissertations Collection

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