Peptide-functionalized oxime hydrogels with tunable mechanical properties and gelation behavior.
We demonstrate the formation of polyethylene glycol (PEG) based hydrogels via oxime ligation and the photoinitiated thiol-ene 3D patterning of peptides within the hydrogel matrix postgelation. The gelation process and final mechanical strength of the hydrogels can be tuned using pH and the catalyst concentration. The time scale to reach the gel point and complete gelation can be shortened from hours to seconds using both pH and aniline catalyst, which facilitates the tuning of the storage modulus from 0.3 to over 15 kPa. Azide- and alkene-functionalized hydrogels were also synthesized, and we have shown the post gelation "click"-type Huisgen 1,3 cycloaddition and thiolene-based radical reactions for spatially defined peptide incorporation. These materials are the initial demonstration for translationally relevant hydrogel materials that possess tunable mechanical regimes attractive to soft tissue engineering and possess atom neutral chemistries attractive for post gelation patterning in the presence or absence of cells.
Departments of †Polymer Science and ‡Chemistry, The University of Akron , Akron, Ohio 44325, United States.
Fei
F
Lin
Jiayi
J
Yu
Wen
W
Tang
Jukuan
J
Zheng
Adrian
A
Defante
Kai
K
Guo
Chrys
C
Wesdemiotis
Matthew L
ML
Becker
D005782:Gels / Q000138:chemical synthesis* / Q000737:chemistry; D020100:Hydrogels / Q000138:chemical synthesis / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration; D015394:Molecular Structure; D010091:Oximes / Q000737:chemistry*; D010316:Particle Size; D010455:Peptides / Q000737:chemistry*; D011092:Polyethylene Glycols / Q000138:chemical synthesis / Q000737:chemistry; D013438:Sulfhydryl Compounds / Q000737:chemistry; D013499:Surface Properties
D005782:Gels; D020100:Hydrogels; D010091:Oximes; D010455:Peptides; D013438:Sulfhydryl Compounds; D011092:Polyethylene Glycols