Solvent Mediating the in Situ Self-Assembly of Polysaccharides for 3D Printing Biomimetic Tissue Scaffolds

Intensively studied 3D printing technology is frequently hindered by the effective printable ink preparation method. Herein, we propose an elegant and gentle solvent consumption strategy to slowly disrupt the thermodynamic stability of the biopolymer (polysaccharide: cellulose, chitin, and chitosan) solution to slightly induce the molecule chains to in situ self-assemble into nanostructures for regulating the rheological properties, eventually achieving the acceptable printability. The polysaccharides are dissolved in the alkali/urea solvent. The weak Lewis acid fumed silica (as solvent mediator) is used to (i) slowly and partially consume the alkali/urea solvent to induce the polysaccharide chains to self-assemble into nanofibers to form a percolating network in a limited scale without leading to gelation and (ii) act as the support to increase the solution modulus, for achieving superior printability and scaffold design flexibility. As a demonstration, the resulting polysaccharide scaffolds with biomimetic nanofibrous structures exhibit superior performances in both the cell-free and cell-loaded bone tissue engineering strategies, showing the potential in tissue engineering. Moreover, the fumed silica could be completely removed by alkali treatment without defecting the nanofibrous structure, showing the potential in various applications. We anticipate our solvent-mediated 3D printing ink preparation concept could be used to fabricate other polymeric facile inks and for widespread applications in diverse fields.