| Summary: | The present study provides a fundamental understanding of the mechanism of action of special new phosphate glass (P-glass) systems, having different glass transition temperatures (<i>T</i><sub>g</sub>), in polyamide 66 (PA66). Dynamic mechanical analysis (DMA) revealed that the <i>T</i><sub>g</sub> of PA66/low <i>T</i><sub>g</sub> P-glass (ILT-1) was significantly shifted to a lower <i>T</i><sub>g</sub> (65 °C), and another transition appeared at high temperature (166 °C). This was supported by a drop in the melting point and the crystallinity of the PA66/ILT-1 hybrid material as detected by differential scanning calorimetry (DSC). The dielectric spectroscopic investigation on the networks’ molecular level structural variations (<i>T</i><sub>g</sub> and sub-<i>T</i><sub>g</sub> relaxations) agreed very well with the DMA and DSC findings. Contrary to intermediate <i>T</i><sub>g</sub>(IIT-3) and high <i>T</i><sub>g</sub> P-glass (IHT-1) based materials, the PA66/ILT-1 hybrid material showed an evidence of splitting the PA66 <i>T</i><sub>g</sub> relaxations into two peaks, thus confirming a strong interaction between PA66 and ILT-1 (low <i>T</i><sub>g</sub> P-glass). Nevertheless, the three different P-glass compositions did not show any effect on the PA66 sub-<i>T</i><sub>g</sub> relaxations (related to the –NH<sub>2</sub> and –OH chain end groups’ motion).
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