Swelling equilibrium of dentin adhesive polymers formed on the water–adhesive phase boundary: Experiments and micromechanical model

During their application to the wet, oral environment, dentin adhesives can experience phase separation and composition change, which can compromise the quality of the hybrid layer formed at the dentin–adhesive interface. The chemical composition of polymer phases formed in the hybrid layer can be represented using a ternary water–adhesive phase diagram. In this paper, these polymer phases are characterized using a suite of mechanical tests and swelling experiments. The experimental results were evaluated using a granular micromechanics-based model incorporating poro-mechanical effects and polymer–solvent thermodynamics. The variation in the model parameters and model-predicted polymer properties was studied as a function of composition along the phase boundary. The resulting structure–property correlations provide insight into interactions occurring at the molecular level in the saturated polymer system. These correlations can be used for modeling the mechanical behavior of the hybrid layer, and are expected to aid in the design and improvement of water-compatible dentin adhesive polymers.