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Throughout recent history scientists have struggled to elucidate the biochemical and biophysical mechanisms that guide the assembly of macromolecular structures. The early models of "sub-assembly" or "self assembly" attempted to explain how individual components could interact in a precisely regulated manner to form higher-ordered complex biological structures. Subsequent studies, using viral systems as assembly models, demonstrated how protein-protein and protein-nucleic acid interactions assist in lowering the thermodynamic barriers that typically disfavor assembly.Due to their simplicity, viruses provide an ideal system to investigate the biophysical mechanisms that drive the assembly of complex biological structures. Proper virion assembly requires numerous macromolecular interactions that proceed along an ordered morphogenetic pathway. While structural proteins are incorporated into the final product, morphogenesis is equally dependent upon scaffolding proteins, which are not included in the mature virion. Since the identification of scaffolding proteins in the bacteriophage P22, homologues have been discovered in many systems. Scaffolding proteins play multiple roles during morphogenesis by inducing protein conformational switches and lowering the thermodynamic barriers to promote virion assembly, while ensuring the efficiency and fidelity of the final product.

Structures with well-defined architectures and tailored physical properties can be produced by supramolecular self-assembly of stimuli-sensitive polymeric inclusion complexes consisting of cyclodextrins. Recently, there has been significant interest in the use of double hydrophilic block copolymers to design novel supramolecular nanostructures as these polymers micellize under external stimuli, such as temperature, pH, and complexation. Cyclodextrins (CDs) have the ability to spontaneously complex with water-soluble guest molecules. The complexation of the polymer with CD induces self-assembly of the polymers. In this research, two systems were studied, a PEO-b-PNIPAM/α-CD system and a PPO-b-PMAA/β-CD system. First, the block copolymers were synthesized by ATRP to achieve well-defined monodisperse polymers. The chemical composition of the polymer was determined by NMR and gel permeation chromatography. Then, the microstructure and aggregation behaviour in aqueous solutions were studied using a combination of static and dynamic light scattering, and isothermal titration and differential scanning calorimetric techniques.

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.

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