Combination of cyclic fatigue testing and materials characterisation to investigate ageing of elastomers

Cyclic fatigue testing and elastomer characterisation were combined to study changes in material properties and network structure of elastomers during thermal ageing. Natural rubber containing a typical additive package with carbon black was studied as a model material. The samples were aged at different temperatures in air or under a nitrogen atmosphere. The fatigue life in number of cycles to failure (S-N curves) was determined from force- and displacement-controlled fatigue tests on tensile bar specimens after different thermal ageing times. Changes in mechanical properties and crosslink density were studied by tensile tests, dynamic mechanical analysis, stress relaxation experiments, compression set measurements, swelling measurements and solid-state NMR. Changes in network density during thermal ageing are related to the interplay between the formation of new crosslinks and chain scission. The average molecular mass of the network chains was found to be a suitable parameter for comparing different characterisation methods. An initial decrease in the molecular mass between two crosslinking points due to post-curing is followed by an increase due to chain scission. A similar trend was found for fatigue life in number of cycles to failure (N) in force-controlled fatigue tests: an increase in N for short ageing times is followed by a decrease after longer ageing times.