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The hydrophilic/hydrophobic nature of cellulose is based on its structural anisotropy. Cellulose chains are arranged in a parallel manner and are organized in sheets stabilized by interchain OH–O hydrogen bonds, whereas the stacking of sheets is stabilized by both van der Waals (vdW) dispersion forces and weak CH–O hydrogen bonds. Cellulose has a strong affinity to itself and materials containing hydroxyls, especially water. Based on the preponderance of hydroxyl functional groups, cellulose polymer is very reactive with water. Water molecular smallness promotes the reaction with the cellulose chains and immediately formed hydrogen bonds. Besides that, vdW dispersion forces play an important role between these two reactive entities. They stabilize the cellulose structure according to the considerable cohesive energy in the cellulose network. Hydrogen bonding, electrostatic interactions, and vdW dispersion forces play an important role in determining the cellulose crystal structure during the cellulose-water interactions. As a result of these interactions, the volume of cellulose undergoes a meaningful change expressed not only by an exponential growth in amorphous regions, but also by an expansion in nanocrystalline regions. In addition, the volume change is associated with the swelling material expressed as a weight gain of the cellulose polymer. Molecular modeling using Accelrys Materials Studio allowed us to open a new horizon and is helpful for understanding cellulose-water interactions.

Interaction Effects between Cellulose and Water in Nanocrystalline and Amorphous Regions: A Novel Approach Using Molecular Modeling