Swelling tests and proton spin-spin relaxation time measurements were carried out on the carbon black filled natural rubber vulcanizates which were treated under various conditions of mechanical stimuli. When the sample temperature is suppressed under 100°C throughout the mechanical stimuli, the molecular mobilies of rubber segments in both quasi-glassy phase around carbon black (M-phase) and liquidlike phase (L-phase) apart from the fillers decrease, however, a noticeable change in the fraction of M or L phase is not observed. The results suggest that the packing density of the rubber chain increases, which induces an increase in the apparent network density evaluated from the swelling tests. On the other hand, when the sample temperature is raised up to 160°C during the mechanical stimuli, the chain mobility in both M and L phases increases, and simultaneously the content of M phase increases. However, the change in content is small, which may be responsible for the decrease in packing density of rubber molecules.
View full abstract