The top-down preparation of graphene nanoplatelets (GNPs) from graphite using different processing methods yields GNPs with very different structural and morphological properties. Hitherto, the role the processing history of the precursor graphite has on the resultant GNPs and their efficacy as a functional filler for rubbers is poorly understood, particularly with regard to the formation of an interphase region between the filler and matrix and the mechanical and cure properties of styrene-butadiene rubber (SBR) compounds. Two types of GNPs (GNP1 and GNP2), with distinct morphology, crystallinity, defect density, and lateral dimensions, were incorporated into SBR to investigate the impact of GNP type on filler dispersion, filler-filler, and filler-rubber interactions on the resulting compound performance. The inclusion of GNP2, with higher crystallinity, larger lateral dimensions, and an absence of defects in the form of folds/bends, significantly outperforms GNP1 in terms of bound rubber content, crosslink density, and mechanical properties. The addition of GNP2 to SBR resulted in a 55% increase in modulus at 100% strain, 50% increase in tensile strength, and a 25% increase in elongation at break compared to the carbon black (CB) filled equivalent. This enhanced reinforcement is derived from the formation of an extensive GNP2–GNP2 network and improved filler-rubber interactions. GNP2 was more highly dispersed in the SBR matrix resulting in more effective curing, reduced crack propagation, and enhanced abrasion resistance in comparison to traditional carbon black filled SBR (RCB). This work provides valuable insights into the impact of graphite processing on the structural properties of GNPs and highlights the importance these properties play in reinforcing SBR.
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