title: Augmentation of postswelling surgical sealant potential of adhesive hydrogels.
abstract: Two-component hydrogels formed with star polyethylene glycol amine and linear dextran aldehyde polymers (PEG:dextran) show promise as tissue-specific surgical sealants. However, there is a significant loss of adhesion strength to soft tissues following PEG:dextran swelling, which may limit material ability to appose disjoined tissues and prevent leakage from surgical sites. We covalently incorporated the modified amino acid L-3,4-dihydroxyphenylalanine (L-DOPA) into PEG:dextran to enhance postswelling sealant performance. L-DOPA is an essential component of marine animal adhesive plaques and has been used to confer wet adhesion in synthetic materials. As both PEG:dextran cohesion and adhesion are mediated by aldehyde-amine interactions, L-DOPA side-groups make it a potent network modulator with potential to affect multiple material properties. Following 1-h submersion in aqueous media, PEG:dextran doped with 3 mM L-DOPA/M aldehyde on average swelled 50.3% less, had 287.4% greater stiffness, and had 53.6% greater functional adhesion strength compared to the neat hydrogel. Increased concentrations of L-DOPA up to 11 mM L-DOPA/M aldehyde similarly curtailed swelling and mitigated property loss with hydration, but sacrificed initial functional adhesion strength, material modulus, and biocompatibility. Taken together, these data support tailored L-DOPA conjugation as a promising approach to enhance the clinical performance of PEG:dextran sealants.
authors.affiliation: Harvard-MIT Division of Health Sciences and Technology, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA. shazly@mit.edu
authors.forename: Tarek M
authors.initials: TM
authors.lastname: Shazly
authors.forename: Aaron B
authors.initials: AB
authors.lastname: Baker
authors.forename: John R
authors.initials: JR
authors.lastname: Naber
authors.forename: Adriana
authors.initials: A
authors.lastname: Bon
authors.forename: Krystyn J
authors.initials: KJ
authors.lastname: Van Vliet
authors.forename: Elazer R
authors.initials: ER
authors.lastname: Edelman
mesh_terms: D000818:Animals; D001672:Biocompatible Materials / Q000494:pharmacology; D002465:Cell Movement / Q000187:drug effects; D019245:Compressive Strength / Q000187:drug effects; D018093:Gelatinases / Q000378:metabolism; D020100:Hydrogels / Q000494:pharmacology*; D007422:Intestines / Q000187:drug effects / Q000473:pathology; D007980:Levodopa / Q000494:pharmacology; D008264:Macrophages / Q000166:cytology / Q000187:drug effects; D009682:Magnetic Resonance Spectroscopy; D008422:Materials Testing / Q000379:methods*; D051379:Mice; D008970:Molecular Weight; D010084:Oxidation-Reduction / Q000187:drug effects; D019919:Prosthesis Implantation; D011677:Punctures; D051381:Rats; D040521:Subcutaneous Tissue / Q000187:drug effects / Q000201:enzymology; D014014:Tissue Adhesives / Q000494:pharmacology*; D014867:Water
chemical_list: D001672:Biocompatible Materials; D020100:Hydrogels; D014014:Tissue Adhesives; D014867:Water; D007980:Levodopa; D018093:Gelatinases