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.

水凝胶具有复杂的异质结构和组织，使其成为高级结构和化妆品应用的有希望的候选者。淀粉由于其低成本和生物相容性而成为生产水凝胶的有吸引力的材料，但是淀粉水凝胶中的聚合物链的结构动力学尚未得到很好的理解，限制了它们的开发和利用。我们采用了一系列的NMR方法（CPSP / MAS，HR-MAS，HPDEC和WPT-CP）来探测具有广泛物理特性的淀粉水凝胶中的分子迁移率和水动力学。这些方法的见解与整体流变学，热学（DSC）和晶体（PXRD）性能有关。我们第一次报道了高动态淀粉链的存在，表现为存在于水凝胶体系液体组分中的溶剂化部分。我们已经将链的结构迁移程度与整体系统的宏观特性相关联，从而提供了对控制水凝胶组装的结构-功能关系的新见解。