On the strain stiffening and nanofiber orientation of physically crosslinked nanocellulose hydrogels

Abstract

Nanocellulose hydrogels that consist of physically crosslinked nanofibrous networks with large amounts of interstitial water have many potential applications as structural materials in biomedical engineering. Quantifying the relationship between micro/nanostructures and their mechanical responses can provide some guidelines for the high-performance mechanical design of counterparts. To this end, we develop a modified physically based constitutive model for examining the effects of the micro/nanostructures of a nanofibrous network on the strain stiffening behaviors of nanocellulose hydrogels under stretching. In addition to the configurational entropy of cellulose nanofiber and mixing energy of water molecule, this theoretical model is particularly concerned with the contribution of the potential energy of hydrogen bond in a thermodynamics framework. Increasing the physical crosslinks between cellulose nanofibers or decreasing the content of water molecules in a certain range can enhance the strain stiffening behaviors of nanocellulose hydrogels. Relatively long and thin cellulose nanofibers have increased tensile strengths. The theoretical predictions are in good agreement with the relevant experimental results. We propose a fiber orientation model for quantifying the relationship between the nanofiber orientation degree and mechanical stretching. This model provides a theoretical foundation for fabricating anisotropic nanofibrous hydrogels via cold drawing.