Post-Synthesis Topological Editing in Polymer Networks

The mechanical properties of polymer networks and gels are closely tied to their topology, including crosslink density and the distribution of topological defects. In contrast to conventional networks, dynamic networks and gels allow for the rearrangement of bonds, offering possibilities of post-synthesis topological editing. Here, we investigate the evolution of the network topology by studying and directing topological evolution in dynamic networks through both theoretical and particle-based simulations. Using a theoretical model to track topological evolution during bond exchange, we predict "error-correction" behavior in dynamic gels, which is corroborated by independent experimental observations. Building on this insight, reactive particle-based simulations are employed to explore novel strategies for selectively editing network topology. With these models, we further demonstrate how such selective topological changes can modify a material's impact-mitigation capabilities and investigate novel strategies for the selective removal of topological defects from hydrogels. Our work demonstrates that post-synthesis topology editing is a powerful route to achieve desirable network structures and material properties. Beginning with the discovery of defect evolution and establishing a mechanistic understanding of selective topology control, these findings provide a foundation for engineering network materials with programmable and optimized topologies.