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Quantitative Correlation between Bound Water and Mechanical Stress Relaxation in Dehydrated Metal-Coordinate Polymer Networks

Cite this: Chem. Mater. 2022, 34, 23, 10329–10337
Publication Date (Web):November 30, 2022
https://doi.org/10.1021/acs.chemmater.2c01795
Copyright © 2022 American Chemical Society

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    Abstract

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    Dynamic metal-coordinate cross-links impart smart and superior physicochemical properties in their deployments in many biological and artificial metallopolymer networks in various stages of solidification via dehydration. Nonetheless, a quantitative model that describes to what extent the dynamic behaviors of metal-coordinate bond transition from the hydrated to the dehydrated state is missing. In previous work, we have shown that local water binding helps metal-coordinate bonds to maintain their dynamic properties during bulk network dehydration, thereby offering mechanical damping properties to the network deep into the dehydrated solid state. Using mussel-inspired hydrogels with chemically tuned fractions of metal-coordinate cross-links, here, we reveal the direct scaling relationship between the macroscopic relaxation time of the dehydrated network and the amount of microscopic water bound by metal-coordinate cross-links. This quantitative relationship between dehydrated metal-coordinate network mechanics and metal-coordinate cross-link dynamics may help us better understand and emulate the sustainable process of solidification via spatiotemporally controlled dehydration of load-bearing materials on wide display in nature.

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    • Additional information on stress-relaxation analyses, TGA, DTG, Raman spectroscopy, solid-state H NMR, rheometry, and quantitative modeling (PDF)

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