We report the reactive layer-by-layer assembly of amine-reactive polymer multilayers using an azlactone-functionalized polymer and small-molecule diamine linkers. This approach yields cross-linked polymer/linker-type films that can be further functionalized, after fabrication, by treatment with functional primary amines, and provides opportunities to incorporate other useful functionality that can be difficult to introduce using other polyamine building blocks. Films fabricated using poly(2-vinyl-4,4-dimethylazlactone) (PVDMA) and three model nondegradable aliphatic diamine linkers yielded reactive thin films that were stable upon incubation in physiologically relevant media. By contrast, films fabricated using PVDMA and varying amounts of the model disulfide-containing diamine linker cystamine were stable in normal physiological media, but were unstable and eroded rapidly upon exposure to chemical reducing agents. We demonstrate that this approach can be used to fabricate functionalized polymer microcapsules that degrade in reducing environments, and that rates of erosion, extents of capsule swelling, and capsule degradation can be tuned by control over the relative concentration of cystamine linker used during fabrication. The polymer/linker approach used here expands the range of properties and functions that can be designed into reactive PVDMA-based coatings, including functionality that can degrade, erode, and undergo triggered destruction in aqueous environments. We therefore anticipate that these approaches will be useful for the functionalization, patterning, and customization of coatings, membranes, capsules, and interfaces of potential utility in biotechnical or biomedical contexts and other areas where degradation and transience are desired. The proof of concept strategies reported here are likely to be general, and should prove useful for the design of amine-reactive coatings containing other functional structures by judicious control of the structures of the linkers used during assembly.

译文

我们报告了使用氮内酯官能化聚合物和小分子二胺接头的胺反应性聚合物多层反应的逐层组装。这种方法产生交联的聚合物/接头型膜,该膜在制造后可以通过用功能性伯胺处理而进一步官能化,并且提供了掺入其他有用的功能的机会,这些功能可能难以使用其他多胺构建模块引入。使用聚 (2-乙烯基-4,4-二甲基氮杂内酯) (PVDMA) 和三种模型不可降解的脂肪族二胺接头制备的薄膜产生的反应性薄膜在生理相关介质中孵育后稳定。相比之下,使用PVDMA和不同量的模型含二硫键的二胺接头cystamine制备的薄膜在正常生理介质中是稳定的,但在暴露于化学还原剂后会迅速腐蚀且不稳定。我们证明了这种方法可用于制造在还原环境中降解的官能化聚合物微胶囊,并且可以通过控制制造过程中使用的胱胺接头的相对浓度来调节侵蚀速率,胶囊溶胀程度和胶囊降解。此处使用的聚合物/接头方法扩展了可设计为基于反应性PVDMA的涂层的性能和功能的范围,包括可在水性环境中降解,侵蚀和遭受触发破坏的功能。因此,我们预计这些方法将有助于在生物技术或生物医学环境以及其他需要降解和瞬态的领域中潜在用途的涂层,膜,胶囊和界面的功能化,图案化和定制。此处报告的概念验证策略可能是一般性的,并且应通过明智地控制组装过程中使用的连接体的结构来证明对包含其他功能结构的胺反应性涂层的设计有用。

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