Shear Deterioration of the Hierarchical Structure of Cellulose Microfibrils under Water Condition: All-Atom Molecular Dynamics Analysis

This study aims to understand the mechanical properties of cellulose nanofibers (CNFs), a nano-sized material element of woods or plants. We develop all-atom (AA) molecular dynamics models of cellulose microfibrils (CMFs), which are the smallest constituent of CNFs. The models were designed for the process of structural failure or the degradation of a hierarchical material of multiple CMF fibers, due to shear deformation. It was assumed that two CMFs were arranged in parallel and in close contact, either in a vacuum or in water. The CMF models in water were built by surrounding AA-modeled water molecules with a few nanometers. Shear deformation was applied in the axial direction of the CMF or in the direction parallel to molecular sheets. Shear moduli were measured, and they agree with previous experimental and computational values. The presence of water molecules reduced the elastic modulus, because of the behavior of water molecules at the interface between CMFs as a function of temperature. In the inelastic region, the CMF often broke down inside CMFs in a vacuum condition. However, in water environments, two CMFs tend to slip away from each other at the interface. Water molecules act like a lubricant between multiple CMFs and promote smooth sliding.