Doctor of Philosophy (Ph.D.)
Vertically oriented graphene nanosheets (VOGN) synthesized by radio frequency plasma enhanced chemical vapor deposition (RF-PECVD) have been fabricated as electrical double layer capacitors (EDLCs). The relatively open morphology of the films provided good frequency response, but had limited capacitance compared to present day activated carbon EDLCs. The objective of this research was to improve the capacitance of these films to a commercially viable level while maintaining sufficient frequency response for AC filtering. The growth of VOGN on Ni and Al substrates has been studied in this work. The native oxide on Ni was thinned at temperatures above ~600ºC with the oxygen from the surface oxide dissolving into the bulk, thus creating a low resistance ohmic contact that reduced the overall equivalent series resistance (ESR). Aluminum was studied because it is the primary substrate material used in electrolytic capacitors. However, it was much more difficult to work with because of its tenacious surface oxide. The maximum capacitance for a 10-minute VOGN/Ni growth observed was ~260µF/cm2, at temperature 850ºC, at 120 Hz, but the morphology was not very ordered. The best combination of capacitance (~160 µF/cm2) and frequency response (phase angle near -85º up to ~3000 Hz) was grown at 750ºC. The capacitance of VOGN/NI was further improved by using coatings of carbon black by an aerosol spray method. A capacitance of 2.3 mF/cm2 and frequency response phase angle near -90º at 120 Hz was achieved. It is the highest specific capacitance for an EDLC, reported in the literature, to date, suitable for AC filtering. Employing Al as a substrate required a novel method of plasma sputter cleaning of the oxide near the Al melting point (660ºC) and superimposing VOGN growth to prevent further oxidation. Initial results were ~80 µF/cm2 at a temperature of 620ºC with frequency response phase angle near -90º. Modeling of a uniform coating of carbon black (100 nm thick) on this underlying VOGN/Al architecture suggests that a capacitance of near 50 mF/cm2 can be achieved thus making this a potentially viable replacement for electrolytic capacitors. Another approach to commercialization of VOGN/Ni EDLCs has been studied by using a single substrate sheet interdigitated pattern design to create a low volume capacitor. A YAG laser was used to ablate resistance lines in the film resulting in a sinuous, square pattern on a VOGN/Ni coated alumina substrate and utilizing a gel electrolyte to create the EDLC.
© The Author
Premathilake, Dilshan V., "Vertically Oriented Graphene Electric Double Layer Capacitors" (2017). Dissertations, Theses, and Masters Projects. William & Mary. Paper 1516639673.