To explore a better understanding of the features of poly(dimethylsiloxane) (PDMS)/silica nanocomposites as fouling-release coatings, a series of PDMS networks filled with silica nanoparticles synthesized in-situ was investigated using small angle x-ray scattering (SAXS) and dynamical mechanical analysis (DMA). Three hydroxyl-terminated (HT) PDMS with different molecular weights, 18,000, 49,000, and 79,000 g/mole, were considered for preparing the nanocomposites at the various weight ratios: 1, 3, and 5:1 of HT-PDMS to tetraethyl orthosilicate (TEOS) as a precursor to the in-situ formation of the nano-silica particles. Two different TEOS were used regarding their degree of polymerization: monomeric type (n∼1) and oligomeric type (n∼5). The small-scale structure of the silica domains was examined using SAXS while scanning electron microscopy (SEM) was used to investigate the large-scale structures of the silica domains. The SAXS data showed a bicontinuous array of aggregates. In addition, the glass transition and molecular dynamics in the nanocomposites were investigated using DMA. The sample including 20 wt% silica, exhibited two tan δ peaks. One was related to the usual polymer glass transition, while the other, occurring at a higher temperature, was attributed to the glass transitions associated with polymer chains in proximity to silica domains. The mobility of these polymer chains was diminished due to their interactions with the surface of the silica particles. This result demonstrated the existence of two types of physical and chemical interactions between the silica aggregates and PDMS chains.
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