Abstract
Hydrogels have a complex, heterogeneous structure and organisation, making them promising candidates for advanced structural and cosmetics applications. Starch is an attractive material for producing hydrogels due to its low cost and biocompatibility, but the structural dynamics of polymer chains within starch hydrogels are not well understood, limiting their development and utilisation. We employed a range of NMR methodologies (CPSP/MAS, HR-MAS, HPDEC and WPT-CP) to probe the molecular mobility and water dynamics within starch hydrogels featuring a wide range of physical properties. The insights from these methods were related to bulk rheological, thermal (DSC) and crystalline (PXRD) properties. We have reported for the first time the presence of highly dynamic starch chains, behaving as solvated moieties existing in the liquid component of hydrogel systems. We have correlated the chains’ degree of structural mobility with macroscopic properties of the bulk systems, providing new insights into the structure-function relationships governing hydrogel assemblies.
Highlights
Hydrogels are a group of materials comprised of cross-linked hydrophilic polymers forming a large network structure, enabling them to hold large amounts of water and/or other biological fluids within their three-dimensional network (Spagnol et al, 2012)
We report the existence of inherent mobile fractions within maize starch hydrogels, the magnitude of which appears to be negatively correlated with their amylose/amylopectin ratio and their rheological strength and structural rigidity
In this work we selected of group of maize starches, which we used for the hydrothermally preparation of hydrogels with a range amylose and amylopectin content
Summary
Hydrogels are a group of materials comprised of cross-linked hydrophilic polymers forming a large network structure, enabling them to hold large amounts of water and/or other biological fluids within their three-dimensional network (Spagnol et al, 2012). Properties, such as their hydrophilicity, low interfacial tension, adaptability/mouldability, swelling and capillary properties and environmental responsivity, have earned them their place as highly promising candidates for the development of biocompatible scaffolds, implants and “smart” drug delivery materials. Starch is a naturally occurring polymer made up of two high molecular weight, polydisperse [1→4]-α-D-glucose polysaccharides – amylose and amylopectin. The properties of starch depend greatly on the molecular composition and structural organisation of its components, and have a significant impact on the material’s highly diverse applications (Morrison, Tester, Snape, Law, & Gidley, 1995; Tester et al, 2004)
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