Dielectric properties of hexagonal boron nitride polymer nanocomposites

Abstract

There is a growing research interest in polymer nanocomposite materials due to their potential in enhancing dielectric properties. However, a considerable amount of variability exists in the literature regarding the electrical performance of polymer nanocomposites, and therefore the underlying mechanisms underpinning their electrical properties are still far from fully understood. Possible reasons for the existing inconsistencies could be due to different material preparation techniques, different nanoparticle dispersion states, unknown filler content, inconsistent sample storage conditions, and unknown water level content in the samples. Determining the principal factors that dominate the electrical behaviour of polymer nanocomposites could allow engineers to tailor the electrical properties of dielectrics for their specific application. As a result, the work reported in this thesis was mainly set out to explore the factors governing the electrical properties of polymer nanocomposites such that the inconsistencies in the literature can be better understood, and consequently eliminated. This thesis investigated the performance of hexagonal boron nitride (hBN) nanocomposites based on two thermoplastic polymers: polystyrene and polyethylene.

Prior to producing any nanocomposites, the hBN particles were characterised using different techniques. The characterisation primarily revealed that the boron nitride particles are in the hexagonal form and the surface of hBN contains a scarce amount of hydroxyl groups. Polystyrene nanocomposites were prepared containing identical amounts of hBN dispersed in different solvents in an attempt to obtain different dispersion states, as a result of different hBN/solvent interactions. The effect of solvent processing was negligible on the dispersion state of the hBN in the polystyrene; no observable difference in the dispersion and electrical properties was reported although the presence of hBN resulted in a slight increase in the breakdown strength relative to the unfilled polystyrene. A range of polyethylene nanocomposites were produced containing different amounts of hBN to understand the effect of the dispersion or aggregation state of the hBN on the breakdown strength. The results revealed that the nanocomposites, regardless of the morphology, exhibited a monotonic increase in breakdown strength with increasing hBN content from 2 wt % to 30 wt %, while maintaining the low dielectric losses of the unfilled polyethylene. While the hBN was found to have a strong nucleating effect on the polyethylene, it was determined that the local change in morphology was not the cause of the enhanced breakdown strength as both the polyethylene nanocomposites obtained by rapid crystallisation, where the development of spherulites was suppressed, and the amorphous polystyrene nanocomposites, also exhibited an improved breakdown strength. Further experiments indicated that the polyethylene nanocomposites did not absorb any moisture from the environment in ambient conditions, and absorbed a very small amount of water even in the 30 wt % polyethylene/hBN nanocomposite when completely immersed in water. Dielectric spectroscopy measurements revealed that the surface hydroxyl groups on the hBN are most likely located only on the edge surfaces of the hBN rather than basal surfaces. The water was most likely loosely bound to the hBN particles, where local water clusters formed. It was remarkable that a percolating water network was not formed in a nanocomposite consisting of an already percolating hBN network, which was largely attributed to the surface chemistry of hBN. Despite the presence of water in the system, the hBN nanocomposites continued to exhibit an enhanced breakdown strength in comparison to the unfilled polyethylene. Therefore, this thesis demonstrated that the electrical behaviour of polymer nanocomposites is most likely dominated by the surface state of the nanoparticles and how the particles interact with the charge carriers; any other effects due to local morphological changes or nanoparticle dispersion are considered to be secondary reasons for changes in the electrical properties.

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ORCID for Thomas Andritsch: orcid.org/0000-0002-3462-022X

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