Correlation of Surface Morphology and Interfacial Adhesive Behavior between Cellulose Surfaces: Quantitative Measurements in Peak-Force Mode with the Colloidal Probe Technique

[Image: see text] A better understanding of cellulose–cellulose interactions is needed in applications such as paper making and all-cellulose composites. To date, cellulose–cellulose studies have been chemistry-oriented. In these studies, the sample surfaces have been modified with different chemicals and then tested under an atomic force microscope (AFM) using a colloidal probe (CP). Studies of cellulose–cellulose interaction based on sample morphology and mechanical properties have been rare as a result of the complex surface structure and the soft texture of the cellulose. The current surface interaction models, such as the Johnson–Kendall–Roberts (JKR) model in which the studied bodies are assumed to have smooth surfaces, can no longer fully reveal the interfacial behavior between two cellulose surfaces. Therefore, we propose a new type of contact model for rough–rough interaction by dividing the surface contacts into primary and secondary levels. The main idea of the new model is to take into account local individual contact details between rough surfaces. The model considers the effect of the surface topography by including the asperities and valleys on a cellulose sphere used as the colloidal probe in imaging the topography of a cellulose membrane (CM). In addition, the correlation between the surface morphology and adhesion is studied. To verify the importance of including the effect of the surface roughness in contact analysis and validate our hypothesis on the correlation between the surface morphology and adhesion, an extensive set of experiments was performed. In the experiments, a combination of the AFM peak-force mode (PFM) and the CP technique was employed to acquire a massive amount of information on cellulose–cellulose interactions by measuring the adhesion among six CSs of different sizes and a CM.