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Synthesis And Characterization Of Nano-Hybrid Systems With Induced Porosities Via Ice Templation

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Abstract

Inorganic-organic hybrid systems are a class of materials that can combine the properties of each constituent material into novel materials with properties that are enhanced or even obtainable where previously unattainable. At nano length scales, these properties can be enhanced via various nano-effects that enable these materials to be tailorable to specific applications. When ice templating (a technique that induces porosity via a sacrificial ice template) is combined with these nano-hybrid systems, a new class of porous materials becomes available that can be imbued with targeted properties as required by the specific application. This dissertation focuses on using these techniques to synthesize novel materials with prerequisite properties as well as to fabricate nano-hybrid porous systems to be used as intermediate precursor materials. This dissertation will first describe work focused on the catalyst layer in PEM fuel cells. In these fuels cells, there is a classic materials science problem where there is a need for a particular material that can accomplish multiple tasks at once. To synthesize a material with all of the prerequisite properties, traditional nanocomposite techniques were combined with ice templating and a dual in situ reduction technique to produce an interconnected porous nano-hybrid scaffold with electrical conductivity (graphene sheets), ionic conductivity (Nafion) and catalytic platinum nanoparticles. Next, the dissertation will focus on ice templating techniques applied to carbon systems to synthesize hierarchical porous carbon (HPC) materials. This new family of carbon materials has a hierarchical porosity across all three length scales (micro -, meso and macro-) and enable the HPCs to have tunable porosities across all three pore length scales. The consequent material is an open, vascular network of interconnected macropores, whose pore walls are made up of mesopores and micropores. This results in a material with easy ingress/egress to the high surface area (up to 2000+ m2/g) meso/micropores by way of the interconnect ed macroporous network. Finally, initial results of applications for the HPCs will be explored including electric double layer capacitors (EDLCs), Li-sulfur batteries, and scaffolds for CO2 capture. In this regard, the HPCs showed an excellent capability t o be used as effective EDLC electrodes with a maximum charge storage capability of 6 W[MIDDLE DOT]h/kg and a ma ximum power density of 14 kW/kg. When used as a carbon support for a Li -S battery cathode, a charge capacity of roughly 600 mAh/gsulfur at a relatively high charge/discharge rate of 1C was obtained, while maintaining good columbic efficiency (> 85%). The HPCs also demonstrated an exceptional ability when used as scaffolds for amine based CO 2 capture, achieving a maximum CO2 capacity of 4.2 mmol/g.

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2013-08-19

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Ice templating; nano-hybrids; electrochemical converters

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Union Local

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Committee Chair

Giannelis, Emmanuel P

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Disalvo, Francis J
Ober, Christopher Kemper

Degree Discipline

Materials Science and Engineering

Degree Name

Ph. D., Materials Science and Engineering

Degree Level

Doctor of Philosophy

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Government Document

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dissertation or thesis

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