Volume 74A, Issue 1 pp. 104-116
Research Article

Controlled release of tethered molecules via engineered hydrogel degradation: Model development and validation

John W. DuBose

John W. DuBose

Department of Bioengineering, Clemson University, Clemson, South Carolina

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Christopher Cutshall

Christopher Cutshall

Department of Chemical Engineering, Clemson University, Clemson, South Carolina

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Andrew T. Metters

Corresponding Author

Andrew T. Metters

Department of Bioengineering, Clemson University, Clemson, South Carolina

Department of Chemical Engineering, Clemson University, Clemson, South Carolina

127 Earle Hall, Clemson University, Clemson, SC 29634-0909Search for more papers by this author
First published: 06 June 2005
Citations: 63

Abstract

A statistical-co-kinetic model has been developed to predict effects of hydrolytic or enzymatic degradation on the macroscopic properties of hydrogels formed through Michael-type addition reactions. Important parameters accounted for by the theoretical calculations are bond cleavage kinetics, microstructural network characteristics such as macromer functionality and crosslinking efficiency, and detailed analysis of degradation products. Previous work indicated the validity of this modeling approach for predicting swelling behavior of hydrolytically degradable gels during early stages of degradation and the quantitative dependence of gel degradation on kinetic and structural parameters. The theoretical methodology is extended in the current work to predict release of covalently bound proteins from the network via labile bonds. Release studies of a network-bound fluoroscopic probe allow validation of model degradation parameters and indicate that macromer functionalization and network crosslinking efficiency can be appropriately tailored to achieve desired swelling profiles and protein release rates over the lifetime of the degradable gel. The effects of these network parameters on the timing of gel dissolution and the protein release that occurs during this phase of degradation are also identified, highlighting the utility of the developed model as a comprehensive tool for optimizing degradable hydrogels as matrices for drug delivery and tissue regeneration. © 2005 Wiley Periodicals, Inc. J Biomed Mater Res, 2005

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