Liquid-Behaviors-Assisted Fabrication of Multidimensional Birefringent Materials from Dynamic Hybrid Hydrogels

Liquid-solid transition is a widely used strategy to shape polymeric materials and encode their microstructures. However, it is still challenging to fully exploit liquid behaviors of material precursors. In particular, the dynamic and static liquid behaviors naturally conflict with each other, which makes it difficult to integrate their advantages in the same materials. Here, by utilizing a shear-thinning phenomenon in the dynamic hybrid hydrogels, we achieve a hydrodynamic alignment of cellulose nanocrystals (CNC) and preserve it in the relaxed hydrogel networks due to the much faster relaxation of polymer networks (within 500 s) than CNC after the unloading of external force. During the following drying process, the surface tension of hydrogels further enhances the orientation index of CNC up to 0.872 in confined geometry, and these anisotropic microstructures demonstrate highly tunable birefringence (up to 0.004 14). Due to the presence of the boundaries of dynamic hydrogels, diverse xerogels including fibers, films, and even complex three-dimensional structures with variable anisotropic microstructures can be fabricated without any external molds.