Poroviscoelastic relaxations and rate-dependent adhesion in gelatin

Hydrogels, polymeric networks swollen with water, exhibit time/rate-dependent adhesion due to their poroviscoleastic constitution. In this study, we conducted probe-tack experiments on gelatin and investigated the influence of dwelling times and unloading rates on pull-off forces and work of adhesion. We utilized in situ contact imaging to monitor separation kinematics and interfacial crack velocities. We found that the crack velocities scaled nonlinearly with the unloading rate, in a power law with an exponent of 0.8 and were independent of dwelling time. At maximum unloading rates corresponding to subsonic interfacial crack speeds, we observed an order of magnitude enhancement in the apparent work of adhesion. The enhancement of adhesion and the crack velocities were related by a power law with an exponent of 0.39. The maximum vertical extension during unloading, a measure of crack opening, exhibited linear correlation with the enhancement of adhesion. Both correlations were in line with the rate-dependent work of fracture modeled for viscoelastic solids (e.g., Persson and Brener model). We explored the links between dwelling times corresponding to varying degrees of poroelastic diffusion and the adhesion. We found 40% additional enhancement in adhesion at the highest unloading rate. This enhancement is due to the unbalanced osmotic pressure, also known as the suction effect. The influence of dwelling times on adhesion was negligible for the interfacial cracks propagating slower than the diffusive time scales. These results identify viscoelastic relaxations as the dominant mechanism governing the rate-dependent enhancement of adhesion, and hence pave the way for tuning rate-dependent adhesion in soft multiphasic materials.