Cellulose nanofibrils (CNFs) obtained by aqueous counter collision (ACC) methods have amphiphilic Janus-type properties, which appear markedly for ACC–CNFs prepared from bacterial nanocellulose (BNC) pellicles. The amphiphilic Janus-type surface is exposed because of the mechanism involved in ACC pulverizing of cellulose materials, in which the predominant interactions of the (2 0 0) lattice plane of the cellulose I crystal structure are weak interplanar van der Waals interactions. Such selective cleavage is more likely to occur for highly crystalline BNC. This study focused on alkali-mercerized cellulose samples, which are of lower crystallinity than BNC. The mercerized raw materials were subjected to ACC treatments and their fiber morphologies, crystallinities, and surface properties were compared to those of ACC–CNFs from native samples. In particular, the Wide-angle X-ray diffraction (WAXD) results suggested that the cleavage was most likely to occur at the (1 1 0) plane in nanofibrils derived from cellulose II, unlike (2 0 0) lattice plane for the case of cellulose I. Accordingly, the entire results indicate that the properties of the ACC-treated mercerized CNFs differ greatly from those of conventional ACC–CNFs composed of cellulose I crystalline structure. This is presumably because ACC nanopulverization proceeds depending on the surface structure and crystalline morphology of the raw material.
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