Peroxide-crosslinked EPDMs filled with calcium-carbonate, silica, or carbon-black and unfilled EPDM were prepared at. varying cure time. Spin-spin relaxation time, T
2, for these specimens were measured by a pulsed NMR spectroscopy with Hahn echo method. The decay curve was decomposed into two components, i.e. a short T
2 and a long T
2, which were respectively arising from network molecules and non-network molecules. For all these specimens, with the increase in the apparent crosslinking density, the network and the non-network T
2 became shorter, resulting in the increase in tensile stress at 100% clongation and the decrease in the tensile strength. The higher order structures of calcium- carbonate-filled and silica-filled EPDMs were similar to that of unfilled EPDM. In the case of carbon-black-filled EPDM, however, the network T
2 was found to be longer and the network fraction smaller than those of other specimens, while the apparent crosslinking density increased and the non-network T
2 shorter. Carbon-black reinforcement seemingly did not relate to the higher order structures obtained by pulsed NMR.
The retention of stress under fatigue for all these specimens tended to decrease as the network T
2 became longer. This result suggested the relationships between the fatigue behavior and the molecular mobility of network component.
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