This work investigates the behaviour of elastomeric chains (polybutadienes of identical molecular weight but different microstructures) in the close vicinity of carbon black surfaces in order to attain a better understanding of the structure and properties of interphases. Elastomer±®ller interactions are assessed through the study of the thermal properties and NMR relaxation characteristics of the corresponding materials. Three series of samples were compared: pure polymers, raw polymer±®ller blends (®ller loading ratio: 50 phr) and solvent-extracted blends (so as to get rid of any polymer which is not under the in¯uence of the solid surface). While differential scanning calorimetry points to the existence of an elastomer fraction which is not detected as undergoing the glass transition, ie is strongly immobilized, [ 1 H] high-resolution high-speed magic-angle spinning solid-state NMR provides information on the effect exerted by polymer±®ller interactions on the mobility of the various constitutive species of the macromolecular backbone. A systematic study of the evolution of the spectral lines yielded by the samples indicates that 1,2-polybutadiene moieties have a particular af®nity towards the carbon black surface which suggests the occurrence of speci®c interactions at the elastomer±®ller interface.

This work investigates the behaviour of elastomeric chains (polybutadienes of identical molecular weight but different microstructures) in the close vicinity of carbon black surfaces in order to attain a better understanding of the structure and properties of interphases. Elastomer–filler interactions are assessed through the study of the thermal properties and NMR relaxation characteristics of the corresponding materials. Three series of samples were compared: pure polymers, raw polymer–filler blends (filler loading ratio: 50 phr) and solvent‐extracted blends (so as to get rid of any polymer which is not under the influence of the solid surface). While differential scanning calorimetry points to the existence of an elastomer fraction which is not detected as undergoing the glass transition, ie is strongly immobilized, [1H] high‐resolution high‐speed magic‐angle spinning solid‐state NMR provides information on the effect exerted by polymer–filler interactions on the mobility of the various constitutive species of the macromolecular backbone. A systematic study of the evolution of the spectral lines yielded by the samples indicates that 1,2‐polybutadiene moieties have a particular affinity towards the carbon black surface which suggests the occurrence of specific interactions at the elastomer–filler interface. © 2001 Society of Chemical Industry

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