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Issue 9, 2014
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Strategies to balance covalent and non-covalent biomolecule attachment within collagen-GAG biomaterials

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Abstract

Strategies to integrate instructive biomolecular signals into a biomaterial are becoming increasingly complex and bioinspired. While a large majority of reports still use repeated treatments with soluble factors, this approach can be prohibitively costly and difficult to translate in vivo for applications where spatial control over signal presentation is necessary. Recent efforts have explored the use of covalent immobilization of biomolecules to the biomaterial, via both bulk (ubiquitous) as well as spatially-selective light-based crosslinking, as a means to both enhance stability and bioactivity. However, little is known about how processing conditions during immobilization impact the degree of unintended non-covalent interactions, or fouling, that takes place between the biomaterial and the biomolecule of interest. Here we demonstrate the impact of processing conditions for bulk carbodiimide (EDC) and photolithography-based benzophenone (BP) crosslinking on specific attachment vs. fouling of a model protein (concanavalin A, ConA) within collagen-glycosaminoglycan (CG) scaffolds. Collagen source significantly impacts the selectivity of biomolecule immobilization. EDC crosslinking intensity and ligand concentration significantly impacted selective immobilization. For benzophenone photoimmobilization we observed that increased UV exposure time leads to increased ConA immobilization. Immobilization efficiency for both EDC and BP strategies was maximal at physiological pH. Increasing ligand concentration during immobilization process led to enhanced immobilization for EDC chemistry, no impact on BP immobilization, but significant increases in non-specific fouling. Given recent efforts to covalently immobilize biomolecules to a biomaterial surface to enhance bioactivity, improved understanding of the impact of crosslinking conditions on selective attachment versus non-specific fouling will inform the design of instructive biomaterials for applications across tissue engineering.

Graphical abstract: Strategies to balance covalent and non-covalent biomolecule attachment within collagen-GAG biomaterials

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Publication details

The article was received on 29 May 2014, accepted on 04 Jul 2014 and first published on 10 Jul 2014


Article type: Paper
DOI: 10.1039/C4BM00193A
Author version available: Download Author version (PDF)
Citation: Biomater. Sci., 2014,2, 1296-1304
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    Strategies to balance covalent and non-covalent biomolecule attachment within collagen-GAG biomaterials

    J. C. Pence, E. A. Gonnerman, R. C. Bailey and B. A. C. Harley, Biomater. Sci., 2014, 2, 1296
    DOI: 10.1039/C4BM00193A

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