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Description
Environmentally responsive microgels have drawn significant attention due to their intrinsic ability to change volume in response to various external stimuli such as pH, temperature, osmotic pressure, or electric and magnetic fields. The extent of particle swelling is controlled by the nature of the polymer-solvent interaction. This thesis focuses on design and synthesis of environmentally responsive microgels and their composites, and encompasses methods of utilizing microgel systems in applications as vehicles for the adsorption, retention, and targeted delivery of chemical species. Furthermore, self-assembled microgel particles at ionic liquid (IL)-water interfaces demonstrate responsive colloidal lattice morphology. The thesis first reports on the fundamental aspects of synthesis, functionalization, and characteristic properties of multifunctional environmentally responsive microgels derived from poly(N-isopropylacrylamide) (PNIPAm) and other functional co-monomers. In particular, the uptake and release of active chemical species such as rheology modifiers into and from these ionic microgels is demonstrated. Moreover, a facile tunable method for the formation of organic-inorganic composites with Fe3O4 nanoparticles adsorbed and embedded within ionic microgel particles is explored. Additionally, the development of zwitterionic microgels (ZI-MG) is presented. These aqueous ZI-MG dispersions exhibit reversible parabolic swelling as a function of pH and display a minimum hydrodynamic diameter at a tunable isoelectric point (IEP). This study also elucidates the controlled uptake and release of surfactants from these particle systems. The extent of surfactant loading and the ensuing relative swelling/deswelling behaviors within the polymer networks are explained in terms of their binding interactions. The latter part of this thesis highlights the versatility of fluorescently labeled microgel particles as stabilizers for IL-water droplets. When the prepared particles form monolayers and equilibrate at the liquid-liquid interface, the colloidal lattice organization may re-order itself depending on the surface charge of these particles. Finally, it is shown that the spontaneously formed and densely packed layers of microgel particles can be employed for extraction applications, as the interface remains permeable to small active species.
ContributorsChen, Haobo (Author) / Dai, Lenore L (Committee member) / Chen, Kangping (Committee member) / Forzani, Erica (Committee member) / Lind, Mary Laura (Committee member) / Mu, Bin (Committee member) / Arizona State University (Publisher)
Created2015
Description
Portable devices rely on battery systems that contribute largely to the overall device form factor and delay portability due to recharging. Membraneless microfluidic fuel cells are considered as the next generation of portable power sources for their compatibility with higher energy density reactants. Microfluidic fuel cells are potentially cost effective and robust because they use low Reynolds number flow to maintain fuel and oxidant separation instead of ion exchange membranes. However, membraneless fuel cells suffer from poor efficiency due to poor mass transport and Ohmic losses. Current microfluidic fuel cell designs suffer from reactant cross-diffusion and thick boundary layers at the electrode surfaces, which result in a compromise between the cell's power output and fuel utilization. This dissertation presents novel flow field architectures aimed at alleviating the mass transport limitations. The first architecture provides a reactant interface where the reactant diffusive concentration gradients are aligned with the bulk flow, mitigating reactant mixing through diffusion and thus crossover. This cell also uses porous electro-catalysts to improve electrode mass transport which results in higher extraction of reactant energy. The second architecture uses porous electrodes and an inert conductive electrolyte stream between the reactants to enhance the interfacial electrical conductivity and maintain complete reactant separation. This design is stacked hydrodynamically and electrically, analogous to membrane based systems, providing increased reactant utilization and power. These fuel cell architectures decouple the fuel cell's power output from its fuel utilization. The fuel cells are tested over a wide range of conditions including variation of the loads, reactant concentrations, background electrolytes, flow rates, and fuel cell geometries. These experiments show that increasing the fuel cell power output is accomplished by increasing reactant flow rates, electrolyte conductivity, and ionic exchange areas, and by decreasing the spacing between the electrodes. The experimental and theoretical observations presented in this dissertation will aid in the future design and commercialization of a new portable power source, which has the desired attributes of high power output per weight and volume and instant rechargeability.
ContributorsSalloum, Kamil S (Author) / Posner, Jonathan D (Thesis advisor) / Adrian, Ronald (Committee member) / Christen, Jennifer (Committee member) / Phelan, Patrick (Committee member) / Chen, Kangping (Committee member) / Arizona State University (Publisher)
Created2010