Highly Efficient and Environmentally Friendly Fabrication of Robust, Programmable, and Biocompatible Anisotropic, All‐Cellulose, Wrinkle‐Patterned Hydrogels for Cell Alignment

• Published in: Advanced materials (Weinheim) Vol. 31; no. 46; pp. e1904762 - n/a
• Main Authors: Zou, Jie, Wu, Shuangquan, Chen, Jie, Lei, Xiaojuan, Li, Qihua, Yu, Hui, Tang, Shan, Ye, Dongdong
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 01-11-2019
• Subjects: 3T3 Cells; Acids; Alignment; Animals; Anisotropy; Biocompatibility; Biocompatible Materials - chemistry; Biocompatible Materials - pharmacology; Biomass; Biomedical materials; Cell Adhesion - drug effects; Cellulose; Cellulose - chemistry; cellulose hydrogels; Crosslinking; gradient crosslinking; Green Chemistry Technology; Hydrogels; Hydrogels - chemistry; Hydrogels - pharmacology; Intervals; Materials science; Mechanical Phenomena; mechanics simulations; Mice; Nanostructure; Polysaccharides; Stability; Submerging; wrinkled patterns; mechanics simulations; wrinkled patterns; gradient crosslinking; cellulose hydrogels
• ISSN: 0935-9648; 1521-4095
• DOI: 10.1002/adma.201904762

Wrinkled hydrogels from biomass sources are potential structural biomaterials. However, for biorelated applications, engineering scalable, structure‐customized, robust, and biocompatible wrinkled hydrogels with highly oriented nanostructures and controllable intervals is still a challenge. A scalable biomass material, namely cellulose, is reported for customizing anisotropic, all‐cellulose, wrinkle‐patterned hydrogels (AWHs) through an ultrafast, auxiliary force, acid‐induced gradient dual‐crosslinking strategy. Direct immersion of a prestretched cellulose alkaline gel in acid and relaxation within seconds allow quick buildup of a consecutive through‐thickness modulus gradient with acid‐penetration‐directed dual‐crosslinking, confirmed by visual 3D Raman microscopy imaging, which drives the formation of self‐wrinkling structures. Moreover, guided by quantitative mechanics simulations, the structure of AWHs is found to exhibit programmable intervals and aligned nanostructures that differ between ridge and valley regions and can be controlled by tuning the prestretching strain and acid treatment time, and these AWHs successfully induce cell alignment. Thus, a new avenue is opened to fabricate polysaccharide‐derived, programmable, anisotropic, wrinkled hydrogels for use as biomedical materials via a bottom‐up method.
A scalable, structure‐customized, robust, and biocompatible all‐cellulose, wrinkle‐patterned hydrogel is engineered with a highly oriented nanostructure using an ultrafast, auxiliary force, acid‐induced gradient dual‐crosslinking strategy that successfully induces cell alignment. This strategy is environmentally friendly, facile, and highly efficient, enabling fabrication of high‐performance polysaccharide‐based hydrogels using a low carbon footprint method.