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Mesoporous Carbon-based Materials for Alternative Energy Applications

  • Author(s): Cross, Kimberly Michelle
  • Advisor(s): Lu, Yunfeng
  • et al.
Abstract

Increasing concerns for the escalating issues activated by the effect of carbon dioxide emissions on the global climate from extensive use of fossil fuels and the limited amount of fossil resources has led to an in-depth search for alternative energy systems, primarily based on nuclear or renewable energy sources. Recent innovations in the production of more efficient devices for energy harvesting, storage, and conversion are based on the incorporation of nanostructured materials into electrochemical systems. The aforementioned nano-electrochemical energy systems hold particular promise for alternative energy transportation related technologies including fuel cells, hydrogen storage, and electrochemical supercapacitors. In each of these devices, nanostructured materials can be used to increase the surface area where the critical chemical reactions occur within the same volume and mass, thereby increasing the energy density, power density, electrical efficiency, and physical robustness of the system.

Durable corrosion resistant carbon support materials for fuel cells have been designed by adding conductive low cost carbon materials with chemically robust ceramic materials. Since a strict control of the pore size is mandatory to optimize properties for improved performance, chemical activation agents have been utilized as porogens to tune surface areas, pore size distributions, and composition of carbon-based mesoporous materials. Through the use of evaporative self-assembly methods, both randomly disordered and surfactant-templated, ordered carbon-silica nanocomposites have been synthesized with controlled surface area, pore volume, and pore size ranging from 50-800 m2/g, 0.025-0.75 cm3/g, and 2-10 nm, respectively.

Multi-walled carbon nanotubes (MWNTs) ranging from 0.05-1.0 wt. % were added to the aforementioned carbon-silica nanocomposites, which provided an additional increase in surface area and improved conductivity. Initially, a conductivity value of 0.0667 S/cm was measured for the composite without carbon nanotubes and the conductivity value improved by over an order of magnitude to 1 S/cm with the addition of 0.5 wt.% CNTs. Triggered by dispersion issues, the agglomeration of MWNTs during the drying process prevented each nanotube from being loaded over a maximum interfacial area. In order to improve the dispersion of carbon nanotubes within the carbon-silica network, electrospinning was explored as a method to improve the alignment of the carbon nanotubes. The electrospun fibers produced with the highest concentration of MWNTs at 1.0 wt.% produced the largest surface area and electrical conductivity values of 333.36 m2/g and 2.09 S/cm, respectively. Capacitance measurements were calculated to examine if improved conductivity results in higher capacitance values. The best capacitance performance was 148 F/g from a carbon-based mesoporous composite with 0.5 wt. % MWNTs in an aqueous electrolyte with a 2.0 mV/s scan rate. An 80% increase in capacitance occurs with the addition of 0.5 wt. % MWNTs. This is in the range of capacitance values produced by hierarchically ordered mesoporous-microporous carbons, reported at 180 F/g.

Fibrous carbon tubes assembled from hydrofluoric acid etched perylenetetracarboxylic diimide bridged silsesquioxane (PDBS) were capable of hydrogen adsorption on the order of 1.3-2.5 wt. % at 77K. Lastly chemically activated phenol- formaldehyde resins produced microporous carbon with 1500 m3/g surface areas and pore sizes ranging from 0.3-0.5 nm, which has potential for asymmetric super-capacitor electrodes. Judicious control over the composition and pore structure of carbon-based nanocomposites can lead to improved performance of various alternative energy materials.

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