The Use of Model Cellulose Materials for Studying Molecular Interactions at Cellulose Interfaces

[Image: see text] Despite extensive research on biobased and fiber-based materials, fundamental questions regarding the molecular processes governing fiber–fiber interactions remain unanswered. In this study, we introduce a method to examine and clarify molecular interactions within fiber–fiber joints using precisely characterized model materials, i.e., regenerated cellulose gel beads with nanometer-smooth surfaces. By physically modifying these materials and drying them together to create model joints, we can investigate the mechanisms responsible for joining cellulose surfaces and how this affects adhesion in both dry and wet states through precise separation measurements. The findings reveal a subtle balance in the joint formation, influencing the development of nanometer-sized structures at the contact zone and likely inducing built-in stresses in the interphase. This research illustrates how model materials can be tailored to control interactions between cellulose-rich surfaces, laying the groundwork for future high-resolution studies aimed at creating stiff, ductile, and/or tough joints between cellulose surfaces and to allow for the design of high-performance biobased materials.