Exploration of the biomacromolecular interactions of an interpenetrating proteo-saccharide hydrogel network at the mucosal interface
Version of Record online: 1 SEP 2013
Copyright © 2013 Wiley Periodicals, Inc.
Journal of Biomedical Materials Research Part A
Volume 101, Issue 12, pages 3616–3629, December 2013
How to Cite
How to cite this article: 2013. Exploration of the biomacromolecular interactions of an interpenetrating proteo-saccharide hydrogel network at the mucosal interface. J Biomed Mater Res Part A 2013: 101A: 3616–3629., , , , , , , .
- Issue online: 28 OCT 2013
- Version of Record online: 1 SEP 2013
- Manuscript Accepted: 5 FEB 2013
- Manuscript Revised: 1 FEB 2013
- Manuscript Received: 13 SEP 2012
- South African National Research Foundation (NRF)
- Council for Scientific and Industrial Research (CSIR) South Africa
- macromolecular interaction;
- synergistic enhancement in rheology;
- molecular mechanics energy relationships
The relationship between mucin (MUC) and pectin (PEC) was explored in an attempt to understand the biomacromolecular interactions that occur at mucosal surfaces when mucus membranes are exposed to PEC-based materials. These interactions were explored through techniques, such as attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy, SEM imagery of lyophilized MUC–PEC blends, thermodynamic analysis, rheology investigations, and in silico static lattice atomistic simulations using a molecular mechanics energy relationships (MMER) approach. Three types of PEC that had different degrees of esterification and degrees of amidation were investigated at different MUC–PEC mass ratios (1:0, 1:1, 1:4, 1:9, and 0:1). The effect PEG 400 and Ca2 + in the MUC–PEC interactions were also studied. ATR-FTIR spectroscopy revealed broadening and strengthening of FTIR peaks at 3363 cm−1 and between 3000–3650 cm−1 due to stretching vibrations of the –OH, –COOH groups on MUC and PEC as well as the –N–H group on MUC. This suggested significant intra- and inter-molecular H-bonding. Morphologically, MUC-rich scaffolds were porous, thin, and multidirectional compared with the smooth, rigid, and unidirectional PEC-rich scaffolds. The Flory–Huggins interaction parameter (χ12) for all MUC–PEC mass ratios was negative, thus confirming MUC–PEC miscibility and interactions. UV absorbance increased with increasing relative concentration of PEC in the aqueous MUC–PEC dispersions. Furthermore, rheology investigations demonstrated synergistic enhancement in viscosity (η) and dynamic moduli upon the addition of PEG 400 and Ca2 +. MMER analysis revealed several key MUC–PEC interactions that corroborated well with the experimental data. Notably, higher esterification and larger mass ratios of PEC yielded greater MUC–PEC interactions. © 2013 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 101A: 3616–3629, 2013.