Department of Chemical and Biomolecular Engineering, The University of Melbourne, Parkville, Victoria 3010, Australia.
Langmuir. 2011 Mar 1;27(5):1724-30. doi: 10.1021/la104510e. Epub 2011 Jan 18.
Nanoengineered poly(methacrylic acid) hydrogel capsules (PMA HCs) are promising candidate carriers for biomedical applications, especially in the areas of drug delivery, encapsulated catalysis, and cell mimicry. The assembly, stability, and degradation of these carriers, as well as their use for the encapsulation of therapeutics, have received considerable attention. However, tailoring the permeability properties of PMA HCs to various types of cargo remains largely unexplored. Herein, we investigate fundamental parameters that govern the structural integrity and the capability of PMA HCs to encapsulate macromolecular cargo. The thiol content of the constituent polymers and the number of deposited polymer layers are shown to be key factors in controlling cargo retention within the PMA HCs. We further introduce a new strategy to achieve disulfide cross-linking for PMA HCs via a thiol-disulfide exchange in order to obtain capsules with superior cargo retention characteristics. Finally, we provide evidence for the semipermeable nature of PMA HCs based on the charge of the solutes and demonstrate that rational design of these systems can yield capsules with specific cargo retention properties. This work contributes toward the development of multilayered polymer capsules and PMA HCs and associated applications in biomedicine.
纳米工程聚（甲基丙烯酸）水凝胶胶囊（PMA HCs）是生物医学应用的有前途的候选载体，特别是在药物输送、封装催化和细胞模拟领域。这些载体的组装、稳定性和降解以及它们在治疗药物封装中的应用受到了相当多的关注。然而，定制 PMA HCs 的渗透性以适应各种类型的货物在很大程度上仍未得到探索。在此，我们研究了控制 PMA HCs 结构完整性和封装大分子货物能力的基本参数。结果表明，组成聚合物的巯基含量和沉积的聚合物层数是控制 PMA HCs 内货物保留的关键因素。我们进一步引入了一种通过硫醇-二硫键交换实现 PMA HCs 二硫键交联的新策略，以获得具有优异货物保留特性的胶囊。最后，我们根据溶质的电荷为 PMA HCs 的半透性提供了证据，并证明了这些系统的合理设计可以产生具有特定货物保留特性的胶囊。这项工作为多层聚合物胶囊和 PMA HCs 的发展以及它们在生物医学中的相关应用做出了贡献。
