Parameters governing strain induced crystallization in filled natural rubber

A series of in situ synchrotron X-ray diffraction experiments are performed during the stretching of weakly and highly vulcanized carbon black (CB), silica and grafted silica filled natural rubber sample (NR). Conversely to literature, Mullins effect observed after one stretching cycle modifies the strain induced crystallization (SIC) behaviour of the sample. The onset of crystallization is ruled by the strain amplification induced by the filler presence. Moreover, fillers (CB and silica) behave as additional crosslinks into NR network, through filler-rubber interactions that either accelerate or slow down the crystallization rate depending on NR matrix chemical crosslink density. This is consistent with the assumption that effective network density, which is due to chemical crosslinks, entanglements, and filler-rubber interactions, controls the crystallization rate.