Department of Physical Chemistry and Materials Science, Faculty of Chemical Technology and Biotechnology, Budapest University of Technology and Economics, Műegyetem rkp. 3., H-1111 Budapest, Hungary.
Laboratory of Interfaces and Nanostructures, Institute of Chemistry, Eötvös Loránd University, Pázmány Péter Sétány 1/A, H-1117 Budapest, Hungary; MTA-TTK Lendület "Momentum" Peptide-Based Vaccines Research Group, Institute of Materials and Environmental Chemistry, Research Centre for Natural Sciences, Magyar Tudósok Krt. 2., H-1117 Budapest, Hungary.
Int J Biol Macromol. 2023 Dec 31;253(Pt 5):126826. doi: 10.1016/j.ijbiomac.2023.126826. Epub 2023 Sep 11.
The type and concentration of charged groups in polymers have a key role in mucoadhesive interactions. A series of cationic poly(amino acid)s with different charge densities was designed to unravel the correlation between chemical structure and mucin-polymer interactions. Colloidal interactions between the mucin protein and synthetic polyaspartamides were tested by dynamic light scattering, zeta potential measurements and turbidimetric titration as a function of polymer-to-mucin mass ratio. The mucoadhesive interactions displayed a strongly non-linear change with polymer composition. The attractive interactions between mucin and the polyaspartamides with at least 50 % cationic groups caused increased light scattering of dispersions due to the aggregation of mucin particles upon their charge reversal. Interactions were further analysed in a thin mucin layer to model life-like situations using a quartz crystal microbalance (QCM) in flow mode. Results pointed out that the fully cationic polyaspartamide is not necessarily superior to derivatives with lower cationic group content. The maximum of adsorbed mass of polymers on mucin was experienced at medium cationic group contents. This emphasizes the relevance of cationic polyaspartamides as mucoadhesive excipients due to their multiple functionalities and the possibility of fine-tuning their interactions with mucin via straightforward chemical steps.
聚合物中带电荷基团的类型和浓度在黏附相互作用中起着关键作用。设计了一系列具有不同电荷密度的阳离子型聚（氨基酸），以揭示化学结构与黏蛋白-聚合物相互作用之间的关系。通过动态光散射、Zeta 电位测量和浊度滴定测试了黏蛋白与合成聚天冬氨酸之间的胶体相互作用，作为聚合物与黏蛋白质量比的函数。黏附相互作用随聚合物组成呈现强烈的非线性变化。至少 50%带正电荷的聚天冬氨酸与黏蛋白之间的吸引相互作用导致分散体的光散射增加，这是由于黏蛋白颗粒在其电荷反转时聚集所致。使用流动模式下的石英晶体微天平 (QCM) 在薄的黏蛋白层中进一步分析了相互作用，以模拟类似生命的情况。结果表明，完全阳离子型聚天冬氨酸不一定优于带较低正电荷基团含量的衍生物。聚合物在黏蛋白上的最大吸附质量出现在中等正电荷基团含量时。这强调了阳离子型聚天冬氨酸作为黏附性赋形剂的相关性，因为它们具有多种功能，并且可以通过简单的化学步骤精细调整它们与黏蛋白的相互作用。
