Unraveling the Role of Architecture in Polymer-Based Glues for Hydrogels.

We investigate polymers of different architectures as potential candidates for the development of glues for hydrogels. Using a combination of coarse-grained modeling and molecular dynamics simulations, we systematically characterize the link between experimentally tunable parameters and adhesion energy. We find that, for a broad set of parameters, adhesion is controlled almost exclusively by the total amount of glue at the interface and by the glue-hydrogel affinity. Instead, it is largely independent of changes in polymer architecture and size, a conclusion that shines new light on previously observed experimental trends. Additionally, we show that the scaling behavior of the properties we measure can be explained by modeling the glue as an ensemble of ideal, noninteracting, and linear polymer segments. We expect that the fundamental insights herein provided will aid the design of new polymer-based adhesives for hydrogels.