Effects of filler content on non-linear viscoelasticity of high fluorine content fluoroelastomer mixture investigated through large amplitude oscillatory shear tests

Non-linear rheological behaviours of high fluorine content fluoroelastomer (HF-FKM) mixtures with varied carbon black (CB) filling amounts were investigated. Non-linear viscoelastic characteristics of HF-FKM mixture are characterised by large amplitude oscillatory shear (LAOS) tests, correlations between rheological behaviour and CB content were then discussed. Each non-linear viscoelastic parameter of HF-FKM mixture presents a three-stage characteristic with increasing CB content, corresponding to ranges of 0–20 phr, 25–30 phr, and 35–45 phr. Three stages of viscoelasticity characteristics for HF-FKM mixtures were considered to depend on the alteration of CB-elastomer network structure with increasing CB content, corresponding to the states where continuous phase of gum, CB-elastomer mesophase and excessive CB agglomerates predominate in mixture compound, respectively. After vulcanisation, samples with 30 phr CB content show the best resilience performance against thermal ageing, contributing to the existence of CB-elastomer mesophase. Samples with 25 phr CB content possess the second lowest compression sets at 225 and 250 °C ageing conditions but perform no better than those with 35 phr at 275 °C. The reason is presumed to be that the presence of excessive CB agglomerates in HF-FKM vulcanisate reduced irreversible deformation of the CB-elastomer network under compression at elevated temperatures.