The Effect of Zeolite Morphology and Loading on the Local Segmental Dynamics and Crystallisation Behaviour of PDMS–Zeolite Composites

The local segmental mobility of polymer chains in polydimethylsiloxane (PDMS) plays a critical role in determining the material's behaviour. Incorporation of zeolite particles can modify these local dynamics, which is crucial as they affect the overall performance of the resulting composite material with potential for various industrial applications. The aim of this study was to investigate the influence of zeolite addition on the local dynamic behaviour of PDMS chain segments in PDMS-zeolite composites. To investigate the effect of zeolite morphology and loading on the segmental dynamics and phase behaviour of PDMS, Zeolite A (with cubic and spherical morphologies) and Zeolite X were incorporated into the PDMS matrix at 20, 30, and 40 wt%. The electron spin resonance (ESR)-spin probe method was used to study molecular dynamics, while the thermal behaviour was analysed using differential scanning calorimetry (DSC). ESR results revealed that the presence of zeolites increases the isothermal crystallisation rate affecting segmental mobility in the amorphous phase below the crystallisation temperature. This effect was found to depend more strongly on zeolite morphology than on filler content. DSC measurements showed no change in glass transition temperature with the addition of zeolite; however, shifts in cold crystallisation and melting behaviour were observed, indicating changes in crystal structure and its degree of perfection. These findings suggest that zeolites act as heterogeneous nucleation agents, with their structural properties playing a critical role in the crystallisation behaviour of PDMS.