Importance of Substrate Functionality on the Adhesion and Debonding of a Pressure-Sensitive Adhesive under Water

We investigate the effect of an aqueous environment on the adhesion of a model acrylic pressure-sensitive adhesive (PSA) composed of 2-ethylhexyl acrylate-co-acrylic acid. We use probe-tack adhesion measurements accompanied by in situ imaging of the contact region during bonding and debonding. Within the probe-tack tests, we use both hydrophilic (piranha and plasma treatment) and hydrophobic (C₁₈-silanization) surface treatments to investigate the contribution of the probe's surface energy on the underwater adhesion. In examining contact formation in air and underwater, we find that the presence of water when contact is made leads to different modes of PSA relaxation and contact formation. For all probes investigated, the adhesive strength between the PSA and the probe decreases when measured underwater. Additionally, we observe that the presence of water during debonding has a more pronounced effect on the adhesive strength of the PSA when probed by a hydrophilic surface as opposed to a hydrophobic surface. Using fingering wavelength analysis, we estimate the surface energy of the PSA in situ and find that when submerged in water, the PSA has a significantly higher surface energy compared to in air. Therefore, combining the observation of different modes of contact formation, the increase in surface energy, and the importance of the surface energy of the probe, we suggest that the decrease in adhesive strength in water can be explained by the hydration of the PSA and by trapped water defects between the PSA and the probe.