Abstract

AbstractCellulose whiskers have been used as reinforcement in a copolymer matrix prepared from a latex phase. If a water suspension‐mixing procedure is adopted, the fibril breakage that usually occurs during the mixing with a molten polymer can be avoided, and an enhanced filler dispersion can be expected. In this study, different processing methods have been used to prepare composite films, either by film casting (water evaporation) or by freeze drying, followed by classical compression or extrusion processes. The thermomechanical properties of these nanocomposites have been investigated, and the influence of processing conditions and the effect of whisker content have been considered. Processing conditions have a large influence on the mechanical behavior and can be classified in ascending order of their reinforcement efficiency: It can be attributed to a decrease of the apparent whisker aspect ratio, due to gradual breakage and/or orientation of the whiskers when hot pressing or extrusion is used. Below Tg, good agreement is found between experimental moduli and the theoretical predictions of the Halpin‐Kardos equation. On the other hand, above Tg, a spectacular reinforcing effect is observed, which is widely underestimated by this short fiber composite model. This is related to the presence of a rigid cellulose network, linked by hydrogen bonds, when the whisker content is above its percolation threshold. The quality of this network (i.e., density and homogeneity) and thus, the magnitude of the reinforcing effect, depend on processing conditions.

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