Abstract
Biological organic-inorganic materials remain a popular source of inspiration for bioinspired materials design and engineering. Inspired by the self-assembling metal-reinforced mussel holdfast threads, we tested if metal-coordinate polymer networks can be utilized as simple composite scaffolds for direct in situ crosslink mineralization. Starting with aqueous solutions of polymers end-functionalized with metal-coordinating ligands of catechol or histidine, here we show that inter-molecular metal-ion coordination complexes can serve as mineral nucleation sites, whereby significant mechanical reinforcement is achieved upon nanoscale particle growth directly at the metal-coordinate network crosslink sites.
Highlights
Biological organic-inorganic materials remain a popular source of inspiration for bioinspired materials design and engineering
While the Fe-catechol system serves as an ideal platform to test our proof of concept of metal-coordinate crosslink mineralization[15,23,24,25], we further examined if this approach could be extended to different metal-ligand coordination systems using histidine-modified polymers, which bind ions and minerals of nickel or copper
We introduce our findings supporting that metal-ion coordination complexes can serve as direct mineral nucleation sites, whereby significant mechanical reinforcement is achieved upon nanoscale particle growth directly at the metalcoordinate network crosslink sites
Summary
Biological organic-inorganic materials remain a popular source of inspiration for bioinspired materials design and engineering. In an attempt to gain deeper insights on the coupling between early stage mineral growth dynamics and polymer network mechanics, we sought to nucleate metal oxide particle growth directly at chain-end inter-molecular crosslinking sites in a model hydrogel scaffold. To assemble such a system, we took inspiration from the incorporation of Fe-catechol coordinate crosslinks in mussel holdfast threads, a material design principle, which have been widely utilized in the integration of tunable stimuli-responsive motifs in advanced hydrogel engineering[10,11,12]. We introduce our findings supporting that metal-ion coordination complexes can serve as direct mineral nucleation sites, whereby significant mechanical reinforcement is achieved upon nanoscale particle growth directly at the metalcoordinate network crosslink sites
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