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Biomacromolecules. 2018 Apr 9;19(4):1276-1284. doi: 10.1021/acs.biomac.8b00100. Epub 2018 Mar 13.

Patterning of Structurally Anisotropic Composite Hydrogel Sheets.

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Department of Chemistry , University of Toronto , 80 Saint George Street , Toronto , Ontario Canada , M5S 3H6.
Department of Chemical Engineering , McMaster University , 1280 Main Street West , Hamilton , Ontario Canada , L8S 4L7.
Institute of Biomaterials and Biomedical Engineering , University of Toronto , 4 Taddle Creek Road , Toronto , Ontario Canada , M5S 3H6.
Department of Chemical Engineering and Applied Chemistry , University of Toronto , 200 College Street , Toronto , Ontario Canada , M5S 3H6.


Compositional and structural patterns play a crucial role in the function of many biological tissues. In the present work, for nanofibrillar hydrogels formed by chemically cross-linked cellulose nanocrystals (CNC) and gelatin, we report a microextrusion-based 3D printing method to generate structurally anisotropic hydrogel sheets with CNCs aligned in the direction of extrusion. We prepared hydrogels with a uniform composition, as well as hydrogels with two different types of compositional gradients. In the first type of gradient hydrogel, the composition of the sheet varied parallel to the direction of CNC alignment. In the second hydrogel type, the composition of the sheet changed orthogonally to the direction of CNC alignment. The hydrogels exhibited gradients in structure, mechanical properties, and permeability, all governed by the compositional patterns, as well as cytocompatibility. These hydrogels have promising applications for both fundamental research and for tissue engineering and regenerative medicine.

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