The effect of water absorption on the dielectric properties of epoxy nanocomposites

In this research, the influence of water absorption on the dielectric properties of epoxy resin and epoxy micro-composites and nano-composites filled with silica has been studied. Nanocomposites were found to absorb significantly more water than unfilled epoxy. However, the microcomposite absorbed less water than unfilled epoxy: corresponding to reduced proportion of the epoxy in this composite. The glass transition temperatures of all the samples were measured by both differential scanning calorimetry and dielectric spectroscopy. The Tg decreased as the water absorption increased and, in all cases, corresponded to a drop of approximately 20K as the humidity was increased from 0% to 100%. This implied that for all the samples, the amount of water in the resin component of the composites was almost identical. It was concluded that the extra water found in the nanocomposites was located around the surface of the nanoparticles. This was confirmed by measuring the water uptake, and the swelling and density change, as a function of humidity as water was absorbed. The water shell model, originally proposed by Lewis and developed by Tanaka, has been further developed to explain low frequency dielectric spectroscopy results in which percolation of charge carriers through overlapping water shells was shown to occur. This has been discussed in terms of a percolation model. At 100% relative humidity, water is believed to surround the nanoparticles to a depth of approximately 5 monolayers. A second layer of water is proposed that is dispersed by sufficiently concentrated to be conductive; this may extend for approximately 25 nm. If all the water had existed in a single layer surrounding a nanoparticle, this layer would have been approximately 3 to 4 nm thick at 100%. This "characteristic thickness" of water surrounding a given size of nanoparticle appeared to be independent of the concentration of nanoparticles but approximately proportional to water uptake. Filler particles that have surfaces that are functionalized to be hydrophobic considerably reduce the amount of water absorbed in nanocomposites under the same conditions of humidity. Comments are made on the possible effect on electrical aging

A "water shell" model for the dielectric properties of hydrated silica-filled epoxy nano-composites

The electrical properties of epoxy resin have been studied as a function of hydration. The epoxy was studied in an un-filled state, filled with 40 µm SiO2 particles, and filled with 50 nm SiO2 particles. The relative humidity was controlled by saturated salt solutions at ambient temperatures from 298-353 K. Measurements were made using dielectric spectroscopy over the frequency range 10-3-105 Hz. The hydration isotherm (i.e. the mass uptake of water) was established by measuring the mass as a function of relative humidity (RH). It was found that the nanocomposites absorb up to 60% more water than the unfilled and micro-filled epoxies. Dielectric spectroscopy shows different conduction and quasi-DC behaviours at very low frequencies (<10-2 Hz) with activation energies dependent on the hydration and temperature. These observations have led to the development of a “water shell” model to explain this phenomenon