Control and Prediction of Gelation Kinetics in Enzymatically Cross-Linked Poly(ethylene glycol) Hydrogels

We demonstrate control of gelation kinetics in formation of poly(ethylene glycol) (PEG) hydrogels by enzymatic cross-linking. A predictive model for gelation kinetics based on macromer structure and composition, stoichiometric ratios of reactants, cross-linking enzyme concentration, and the underlyi...

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Bibliographic Details
Published in:Macromolecules 2000-07, Vol.33 (15), p.5476-5480
Main Authors: Sperinde, Jeffrey J, Griffith, Linda G
Format: Article
Language:English
Subjects:
Applied sciences
Exact sciences and technology
Organic polymers
Physicochemistry of polymers
Polymerization
Preparation, kinetics, thermodynamics, mechanism and catalysts
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Summary:We demonstrate control of gelation kinetics in formation of poly(ethylene glycol) (PEG) hydrogels by enzymatic cross-linking. A predictive model for gelation kinetics based on macromer structure and composition, stoichiometric ratios of reactants, cross-linking enzyme concentration, and the underlying kinetics of enzyme reaction was developed on the basis of classical Flory−Stockmayer theory. Experiments with substrate-functionalized multiarm comb PEG showed good agreement with theory upon variation of the enzyme concentration, with a slight overprediction in the time to gelation. Experiments with a substrate-functionalized difunctional PEG in conjunction with a polypeptide where macromer concentrations were varied were also consistent with theory, but with a slight underprediction of gelation time.
ISSN:0024-9297
1520-5835
DOI:10.1021/ma000459d