The aim of this article was to investigate the effect of a NaA-type zeolite on a polydimethylsiloxane (PDMS)–zeolite composite. The obtained results show that the introduction of a NaA-type zeolite into polysiloxane matrices results in a change of the equilibrium degree of swelling (DSe) of composites in toluene, their hardness, and their thermal stability. With increase in the zeolite, the time required to achieve the DSe is reduced, DSe decreases, and hardness increases. A double effect of the zeolite concentration on the change of the composite characteristics was noted. At zeolite concentrations of up to 20%, there is a drastic change of the DSe and hardness with zeolite concentration, while this effect is considerably less pronounced at higher concentrations. The results obtained show that a NaA-type zeolite plays the role of a reinforcing filler. A new mechanism of bonding the zeolite into the composite was suggested. According to this model, there is a possibility that bonds are established between the polymer and the zeolite via interaction of the π-bond of terminal vinyl groups of PDMS with the Na cation of the zeolite. With increase in the zeolite concentration in the composite, the total number of established polymer–zeolite bonds increases, but the density of the interaction decreases. This explains the change in the characteristics of the composite with the change of zeolite concentration. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 77: 1171–1176, 2000
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