Cellulosic fiber: mechanical fibrillation-morphology-rheology relationships

Abstract This study aims to investigate the relationship between mechanical fibrillation, morphological properties, and rheological behavior of cellulosic fiber. Three types of cellulosic fibers were obtained by adjusting mechanical fibrillation, namely squashed cellulose, incompletely nanofibrillated cellulose, and completely nanofibrillated cellulose, respectively. The squashed cellulose with large size and small aspect ratio had low entanglement capacity, thus forming a weak fiber network. The corresponding suspension exhibited low viscosity, weak elastic behavior, small yield stress, and low dynamic stability. An obviously increasing aspect ratio and entanglement capacity were observed with increasing mechanical fibrillation, resulting in entangled fiber network structure. Hence, the cellulosic fiber suspension obtained by more mechanical fibrillation exhibited higher viscosity, stronger gel-like behavior, and bigger yield stress. Moreover, the extremely entangled fiber network structure has better anti-deformation capacity and recovery capacity. We revealed the fundamental insights into the relationship between morphologies and rheological properties of cellulosic fiber, paving the way for designing cellulose-based materials.