HORIZONS FOR DESIGN OF FILLED RUBBER INFORMED BY MOLECULAR DYNAMICS SIMULATION

SM Smith and DS Simmons, RUBBER CHEMISTRY AND TECHNOLOGY, 90, 238-263 (2017).

DOI: 10.5254/rct.17.82668

Fillers such as carbon black provide a long-standing and essential strategy for the mechanical reinforcement of rubber in tires and other load-bearing applications. Despite their technological importance, however, the microscopic mechanism of this reinforcement remains a matter of considerable debate. A predictive understanding of filler- based reinforcement could catalyze the design of new rubber-filler composites with enhanced performance. Molecular dynamics simulations of rubber mechanical response in the presence of structured fillers offer a new strategy for resolving the origins of filler-based reinforcement and guiding filler design. Results of for ideal rubber-filler dispersions over a range of filler structures suggest that neither hydrodynamic effects nor non-deformable "bound rubber domains" are necessary to achieve high reinforcement. Moreover, simulations show that particle surface area is a poor predictor of reinforcement. Instead, simulated reinforcement correlates strongly with filler structure, with more rarified filler structure predicting much greater reinforcement at fixed loading. Simulation results are consistent with a scenario in which reinforcement at industrially relevant loadings is dominated by formation of a jammed network of filler particles, suggesting that reinforced rubber can be understood as a superposition of two materials: a rubbery solid, and a jammed granular solid. This perspective points to an opportunity to improve filler-reinforced rubber design by leveraging concepts and expertise developed over many decades in the fields of jamming and granular media.

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