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Reversible Control of Gelatin Hydrogel Stiffness by Using DNA Crosslinkers** |
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| Authors: | Alex Buchberger Harpinder Saini Kiarash Rahmani Eliato Azadeh Zare Ryan Merkley Yang Xu Julio Bernal Robert Ros Mehdi Nikkhah Dr Nicholas Stephanopoulos |
| Affiliation: | 1. School of Molecular Sciences, Arizona State University, P.O. Box 877301, Tempe, AZ 85287 USA
Center for Molecular Design and Biomimetics, The Biodesign Institute, Arizona State University, 1001 S. McAllister Ave, Tempe, AZ 85281 USA These authors contributed equally to this work.;2. School of Biological and Health Systems Engineering, Arizona State University, 501 E. Tyler mall, ECG 334A, Tempe AZ, 85287 USA Virginia G. Piper Center for Personalized Diagnostics The Biodesign Institute, Arizona State University, 1001 S. McAllister Ave, Tempe AZ, 85281 USA These authors contributed equally to this work.;3. Department of Physics, Arizona State University, 550 E Tyler Drive, Tempe, AZ 85287 USA Center for Biological Physics, Arizona State University, P.O. Box 871504, Tempe, AZ, 85287 USA Center for Single Molecule Biophysics, The Biodesign Institute, Arizona State University, 1001 S. McAllister Ave, Tempe, AZ 85281 USA These authors contributed equally to this work.;4. Department of Physics, Arizona State University, 550 E Tyler Drive, Tempe, AZ 85287 USA Center for Biological Physics, Arizona State University, P.O. Box 871504, Tempe, AZ, 85287 USA Center for Single Molecule Biophysics, The Biodesign Institute, Arizona State University, 1001 S. McAllister Ave, Tempe, AZ 85281 USA;5. School of Molecular Sciences, Arizona State University, P.O. Box 877301, Tempe, AZ 85287 USA Center for Molecular Design and Biomimetics, The Biodesign Institute, Arizona State University, 1001 S. McAllister Ave, Tempe, AZ 85281 USA;6. Department of Physics, Arizona State University, 550 E Tyler Drive, Tempe, AZ 85287 USA;7. School of Biological and Health Systems Engineering, Arizona State University, 501 E. Tyler mall, ECG 334A, Tempe AZ, 85287 USA;8. School of Molecular Sciences, Arizona State University, P.O. Box 877301, Tempe, AZ 85287 USA |
| Abstract: | Biomaterials with dynamically tunable properties are critical for a range of applications in regenerative medicine and basic biology. In this work, we show the reversible control of gelatin methacrylate (GelMA) hydrogel stiffness through the use of DNA crosslinkers. We replaced some of the inter-GelMA crosslinks with double-stranded DNA, allowing for their removal through toehold-mediated strand displacement. The crosslinks could be restored by adding fresh dsDNA with complementary handles to those on the hydrogel. The elastic modulus (G’) of the hydrogels could be tuned between 500 and 1000 Pa, reversibly, over two cycles without degradation of performance. By functionalizing the gels with a second DNA strand, it was possible to control the crosslink density and a model ligand in an orthogonal fashion with two different displacement strands. Our results demonstrate the potential for DNA to reversibly control both stiffness and ligand presentation in a protein-based hydrogel, and will be useful for teasing apart the spatiotemporal behavior of encapsulated cells. |
| Keywords: | biomaterials DNA dynamic hydrogels self-assembly |