Two Different Surface Properties of Regenerated Cellulose due to Structural Anisotropy

Contact angles of water droplet on regenerated cellulose films as an index of wettability were positively correlated with the orientation of (1-10) crystal planes and crystallinity. Because hydroxyl groups of cellulose are located at the equatorial positions of glucopyranose rings, corresponding to the surface of (1-10) crystal planes, the hydrophilicity of the (1-10) surface is expected to be very high. It is natural, therefore, that higher planar orientation of (1-10) planes and crystallinity lead to higher density of hydroxyl groups on the surface of regenerated cellulose films resulting in higher wettability. In contrast, hydrogen atoms are located at the axial positions of the glucopyranose rings, corresponding to the surface of (110) planes. Thus, the (110) surface is expected to be hydrophobic, and the surface energy obtained by computer simulations was far lower than that of the (1-10) surface. This suggests that cellulose with complementary properties, i.e., hydrophobicity, may be created by structural controls such as reversing the planar orientation from (1-10) to (110). Although it was not possible to reverse this orientation completely, post-treatments with a nonpolar solvent (e.g., hexane), liquid ammonia or hot glycerol can somewhat control the wettability of regenerated cellulose films.