Highly tunable elastomeric silk biomaterials.
Elastomeric, fully degradable and biocompatible biomaterials are rare, with current options presenting significant limitations in terms of ease of functionalization and tunable mechanical and degradation properties. We report a new method for covalently crosslinking tyrosine residues in silk proteins, via horseradish peroxidase and hydrogen peroxide, to generate highly elastic hydrogels with tunable properties. The tunable mechanical properties, gelation kinetics and swelling properties of these new protein polymers, in addition to their ability to withstand shear strains on the order of 100%, compressive strains greater than 70% and display stiffness between 200 - 10,000 Pa, covering a significant portion of the properties of native soft tissues. Molecular weight and solvent composition allowed control of material mechanical properties over several orders of magnitude while maintaining high resilience and resistance to fatigue. Encapsulation of human bone marrow derived mesenchymal stem cells (hMSC) showed long term survival and exhibited cell-matrix interactions reflective of both silk concentration and gelation conditions. Further biocompatibility of these materials were demonstrated within vivoevaluation. These new protein-based elastomeric and degradable hydrogels represent an exciting new biomaterials option, with a unique combination of properties, for tissue engineering and regenerative medicine.
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Benjamin P
BP
Partlow
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Craig W
CW
Hanna
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Jelena
J
Rnjak-Kovacina
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Jodie E
JE
Moreau
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Matthew B
MB
Applegate
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Kelly A
KA
Burke
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Benedetto
B
Marelli
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Alexander N
AN
Mitropoulos
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
Fiorenzo G
FG
Omenetto
Department of Biomedical Engineering, Tufts University, 4 Colby St. Medford, MA 02155 (USA).
David L
DL
Kaplan
biomaterials; biopolymers; elastomers; hydrogels; silk