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Mimicking Dynamic Adhesiveness and Strain Stiffening Behavior of Biological Tissues in Tough and Self-Healable Cellulose Nanocomposite Hydrogels.

Despite self-healing gels with structural resemblance to biological tissues attract great attention in biomedical field, it remains a dilemma for combination between fast self-healing properties and high mechanical toughness. Based on the design of dynamic reversible cross-links, we incorporate rigid tannic acid-coated cellulose nanocrystal (TA@CNC) motifs into the poly(vinyl alcohol) (PVA)-borax dynamic networks for the fabrication of a high toughness and rapidly self-healing nanocomposite (NC) hydrogel, together with dynamically adhesive and strain stiffening properties that are particularly indispensable for practical application in soft tissues substitutes. The results demonstrate that the obtained NC gels present a highly interconnected network, where flexible PVA chains wrap onto the rigid TA@CNC motifs and form the dynamic TA@CNC-PVA clusters associated by hydrogen bonds, affording the critical mechanical toughness. The synergetic interactions between borate-diol bonds and hydrogen bonds impart typical self-healing behavior into the NC gels, allowing the dynamic cross-linked networks undergo fast rearrangement in the time scale of seconds. Moreover, the obtained NC hydrogels not only mimic the main feature of biological tissue with the unique strain stiffening behavior, but also display unique dynamic adhesiveness to nonporous and porous substrates. It is expected that this versatile approach opens up a new prospect for the rational design of multifunctional cellulosic hydrogels with remarkable performance to expand their applications.

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