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The Payne Effect (also known as the Fletcher–Gent Effect) has a fundamental impact on the behavior of filled rubber composites and therefore must be considered during their design. This study investigates the influence of carbon black (CB) surface area and structure on the observed Payne Effect and builds on the existing models of Kraus and Ulmer to explain this phenomenon. Dynamic strain sweeps were carried out on natural rubber (NR) compounds containing eight different grades of CB at equivalent volume fractions. The loss and storage moduli were modeled according to the Kraus and Ulmer equations, using a curve optimization tool in SciPy. Subsequent regression analysis provided strong correlations between the fitting parameters and the CB structure and surface area. Using this regression analysis, this work provides further insight into the physical meaning behind the Kraus and Ulmer models, which are phenomenological in nature. [ABSTRACT FROM AUTHOR]

The influence of carbon black (CB) structure and surface area on key rubber properties such as monotonic stress-strain, cyclic stress–strain, and dynamic mechanical behaviors are investigated in this paper. Natural rubber compounds containing eight different CBs were examined at equivalent particulate volume fractions. The CBs varied in their surface area and structure properties according to a wide experimental design space, allowing robust correlations to the experimental data sets to be extracted. Carbon black structure plays a dominant role in defining the monotonic stress–strain properties (e.g., secant moduli) of the compounds. In line with the previous literature, this is primarily due to strain amplification and occluded rubber mechanisms. For cyclic stress–strain properties, which include the Mullins effect and cyclic softening, the observed mechanical hysteresis is strongly correlated with carbon black structure, which implies that hysteretic energy dissipation at medium to large strain values is isolated in the rubber matrix and arises due to matrix overstrain effects. Under small to medium dynamic strain conditions, classical strain dependence of viscoelastic moduli is observed (the Payne effect), the magnitude of which varies dramatically and systematically depending on the colloidal properties of the CB. At low strain amplitudes, both CB structure and surface area are positively correlated to the complex moduli. Beyond ~2% strain amplitude the effect of surface area vanishes, while structure plays an increasing and eventually dominant role in defining the complex modulus. This transition in colloidal correlations reflects the transition in stiffening mechanisms from flexing of rigid percolated particle networks at low strains to strain amplification at medium to high strains. By rescaling the dynamic mechanical data sets to peak dynamic stress and peak strain energy density, the influence of CB colloidal properties on compound hysteresis under strain, stress, and strain energy density control can be estimated. This has considerable significance for materials selection in rubber product development. [ABSTRACT FROM AUTHOR]

The strain and thermal dependence of the dynamic mechanical properties of carbon black filler networks underpin the performance of many rubber components. These effects are examined by varying the surface energetics of carbon black. This has a profound influence on the level of flocculation of the carbon black network in the final crosslinked compounds. Filler networks comprised of thermally deactivated carbon blacks are significantly more strain-sensitive - shifting the onset of the Payne effect to smaller dynamic strains. Using free vibration equipment to precisely probe the thermal sensitivity of the linear viscoelastic properties of the filled compounds, it is shown that carbon black deactivation results in carbon black networks which are more thermally sensitive than corresponding unmodified carbon black networks. Increased thermal dependence of the dynamic moduli results in the appearance of a secondary increase in tan δ as a function of increasing temperature well above the rubber Tg - which is not correlated with any thermal transitions in calorimetric experiments. Such effects are prevalent in the relevant literature for various rubber-filler combinations but their physical origins are often misinterpreted or unexplained. A rationalization of these effects based on the dynamics of the filler network is presented. [ABSTRACT FROM AUTHOR]