Abstract
Pressure-sensitive adhesion arises at a specific rheological behavior of polymer systems, which should correlate with their relaxation properties, making them potentially useful for predicting and altering adhesive performance. This work systematically studied the rheology of eco-friendly pressure-sensitive adhesives based on non-crosslinked polyisobutylene ternary blends free of solvents and byproducts, which serve for reversible adhesive bonding. The ratio between individual polymer components differing in molecular weight affected the rheological, relaxation, and adhesion properties of the constituted adhesive blends, allowing for their tuning. The viscosity and viscoelasticity of the adhesives were studied using rotational rheometry, while their adhesive bonds with steel were examined by probe tack and shear lap tests at different temperatures. The adhesive bond durability at shear and pull-off detachments depended on the adhesive composition, temperature, and contact time under pressure. The double differentiation of the continuous relaxation spectra of the adhesives enabled the accurate determination of their characteristic relaxation times, which controlled the durability of the adhesive bonds. A universal linear correlation between the reduced failure time of adhesive bonds and their reduced formation time enabled the prediction of their durability with high precision (Pearson correlation coefficient = 0.958, p-value < 0.001) over at least a four-order-of-magnitude time range. The reduction in the formation/failure times of adhesive bonds was most accurately achieved using the longest relaxation time of the adhesives, associated with their highest-molecular-weight polyisobutylene component. Thus, the highest-molecular-weight polymer played a dominant role in adhesive performance, determining both the stress relaxation during the formation of adhesive bonds and their durability under applied load. In turn, this finding enables the prediction and improvement of adhesive bond durability by increasing the bond formation time (a durability rise by up to 10-100 times) and extending the adhesive's longest relaxation time through elevating the molecular weight or proportion of its highest-molecular-weight component (a durability rise by 100-350%).