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The morphology and viscoelastic properties of films prepared from bimodal latex blends containing equal weight fractions of soft and hard latex particles were investigated as a function of the particle sizes and the particle size ratio (soft particle diameter/hard particle diameter). Minimum film formation temperature (MFT) measurements were associated with transmission electron microscopy (TEM) to emphasize the particle size ratio dependence of the film formation properties. A significant increase of the MFT values with the soft/hard particle size ratio was observed. As long as the particle size ratio was low, TEM micrographs showed that the film forming soft particles, undergoing complete coalescence, clearly act as the continuous phase where the non film forming hard particles are found evenly dispersed while keeping their initial spherical shape. At higher values of the particle size ratio, TEM micrographs pointed out that the soft particles are prevented from coming into contact with each other by the surrounding hard particles, therefore dramatically increasing the MFT of the sample and resulting in a non film forming latex blend. The existence of a critical volume fraction of hard particles that is directly related to the soft/hard particle size ratio was then established on the basis of geometrical arguments involving the percolation theory. The higher the particle size ratio, the lower the critical volume fraction of hard particles that leads to a macroscopic phase inversion resulting in a non film forming bimodal latex blend. Subsequently, the mechanical film properties were investigated by solid-state dynamic mechanical analysis. The size of the dispersed hard phase was found to affect the final viscoelastic film properties. The smaller the size of the hard particles, the better the mechanical enhancement of the mechanical film properties. Last, the experimental viscoelastic thermograms were compared with some theoretical predictions based on self-consistent mechanical modeling. The final film properties of the bimodal hard/soft latex blends were then directly connected to the film formation properties.

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