The rheological properties of liquid polybutadiene rubber/organo-clay nanocomposite gels were
investigated by rheological experiments, focusing on the effects of clay exfoliation and orientation−disorientation
as well as polymer−clay interaction and temperature. Both irreversible and reversible viscosity transitions were
observed in the temperature range from 26 to 136 °C in steady shear experiments on as-prepared and exfoliated
samples. These transitions depend strongly on the end groups, molecular weight of the liquid rubber, and the
shear field. The irreversible transition is attributed to the exfoliation of the clay, and the reversible transition can
be understood as a shear-induced orientation−disorientation transition of the clay sheets. Polymer−clay interaction
is confirmed to be a key controlling factor of the orientation−disorientation transition, whereas the shear field
plays a critical role to induce such a transition. To our knowledge, this is the first rheological observation of the
in-situ exfoliation process and the shear-induced orientation−disorientation transition of layered silicate in polymer/organo-clay nanocomposites. A tentative model was suggested on the basis of the clay exfoliation and orientation−disorientation transition, and the model is used to explain the observed unique rheological behavior.