Thermoreversible gelation in poly(ethylene oxide)/carbon black hybrid melts

•PEO/CB melts exhibit thermoreversible physical gelation.•At high temperatures particle clustering leads to dramatic rheological enhancements.•When strong matrix-particle interactions are present the gelation is diminished.

The study focuses on the structure and viscoelasticity of poly(ethylene oxide)/carbon black fluids. The hybrids when subjected to extreme thermal annealing (at temperatures far above the melting point of the matrix) exhibit a 3–4 orders of magnitude increase in viscosity. Surprisingly, the effect is reversible and the viscosity reverts back to its initial value upon subsequent cooling. This rather unique sol–gel transition in terms of strength, steepness and thermal reversibility points to major structural rearrangements via extensive particle clustering, in agreement with microscopy observations. In related systems it was found that when matrix-particle electrostatic interactions are present the gelation is essentially diminished.

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