Bio-inspired metal-coordination crosslinking: easy access to broad dynamics when engineering polymer gel mechanics

Efforts to engineer polymer material mechanics is increasingly coupled to the design of transient crosslink dynamics. We have sought to gain a deeper understanding of how polymer gel mechanical properties can be controlled over multiple hierarchical time-scales via design of bio-inspired metal-coordinate crosslink structure on multiple length-scales. By utilizing metal ion-coordination complexes and metal nanoparticle-coordination junctions as supra-molecular crosslink structures, we have gained unique access to network dynamics on the microscopic scale, and thereby opportunities to broadly shape the distribution of network stress relaxation on the macroscopic scale. Our findings offer deeper insights on how to engineer gel stress relaxation mechanics directly via design of supramolecular crosslink structure dynamics, and could help improve our understanding of spatio-temporal molecular hierarchy in loadbearing biological materials.