Hydrogels demonstrate great potential in diverse applications, ranging from glues to biomedical applications. In particular, robust and tough hydrogels have attracted lots of attention in recent years, but many of them were still suffering from the complicated preparation procedures, limited polymer selection and strict control of hydrogel networks.<br/>Herein, a novel type of robust hydrogels with heterogeneous structures based on supermolecular self-assembly with nanocellulose as crosslinkers is presented. Cellulose nanocrystals (CNCs) surface was functionalized with pre-organized dynamic groups. These dynamic groups, such as host-guest cyclodextrin-adamentin or phenylboronic acid-dopamine complex, contain polymerizable groups and will be intergrated in the polymer network during further <i>in situ</i> polymerization. Because of the immobilization of these supramolecular groups at the surface of CNCs, the CNCs act as crosslinkers for stabilizing whole hydrogel networks. Due to the dynamic nature of these dynamic bonds, the extreme contrast in the mechanical properties of rigid nano-crosslinkers and soft flexible polymer phase also creates heterogeneity in stiffness and elastic modulus. The hydrogels showed high toughness as well as stretchability and are favorable to resist fatigue under repeated work cycles. In summary, we designed and introduced a group of dynamic heterogeneous hydrogels with robust and adjustable mechanical properties based on supramolecular self-assembled dynamic bonds on CNCs.<br/>

Robust heterogeneous hydrogels based on supermolecular self-assembly with nanocellulose as dynamic crosslinkers

255th National Meeting (2018)

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