Development of Improved Graphene Production and Three-dimensional Architecture for Application in Electrochemical Capacitors

Abstract

Increasing energy demand makes the development of higher energy storage batteries, imperative. However, one of the major advantages of fossil fuels as an energy source is they can provide variably large quantities of power when desired. This is where electrochemical capacitors can continue to carve out a niche market supplying moderate energy storage, but with high specific power output. However, current issues with carbon precursors necessitate further development. Further, production requires high temperature, energy intensive carbonization to create the active pore sites and develop the pores.

Double-layer capacitive materials researched to replace active carbons generally require properties that include: very high surface area, high pore accessibility and wettability, strong electrical conductivity, structural stability, and optionally reversible functional groups that lend to energy storage through pseudocapacitive mechanisms. In recent years, nanostructured carbon materials which could in future be tailored through bottom up processing have the potential to exhibit favourable properties have also contributed to the growth in this field. This thesis presents research on graphene, an emerging 2-dimensional carbon material. So far, production of graphene in bulk exhibits issues including restacking, structural damage and poor exfoliation. However, the high chemical stability, moderate conductivity and high electroactive behaviour even with moderate exposed surface area makes them an excellent standalone material or a potential support material. Two projects presented focus on enhancing the capacitance through functionality and controlling graphene formation to enhance performance.

The first study addresses graphene enhancement possible with heteroatom functionality, produced by a single step low temperature hydrothermal reduction process. The dopant methodology was successful in adding nitrogen functionality to the reduced graphene oxide basal and the effect of nitrogen type was considered.

The second study addresses the need for greater control of the rGO structure on the macro-scale. By harnessing the change in interactions between the GO intermediate and final rGO sheets we were able to successfully control the assembly of graphene, creating micro and macro-pore order and high capacitive performance. Further, self assembly directly onto the current collector eliminates process steps involved in the production of EDLC electrodes.