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首页> 美国卫生研究院文献>other >Polyelectrolyte Multilayers Fabricated from ‘Charge-Shifting’ Anionic Polymers: A New Approach to Controlled Film Disruption and the Release of Cationic Agents from Surfaces
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Polyelectrolyte Multilayers Fabricated from ‘Charge-Shifting’ Anionic Polymers: A New Approach to Controlled Film Disruption and the Release of Cationic Agents from Surfaces

机译：由电荷转移阴离子聚合物制成的聚电解质多层膜：控制膜破裂和从表面释放阳离子剂的新方法

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We report an approach to the design of ‘charge-shifting’ anionic polymers that provides control over the disruption of ultrathin polyelectrolyte multilayers in aqueous media. We demonstrate that the addition of citraconic anhydride to poly(allylamine) yields an anionic, carboxylate-functionalized polymer (polymer >2) that can be converted readily back to cationic poly(allylamine) in acidic environments. The incorporation of polymer >2 into polyelectrolyte multilayers thus provides an approach to the fabrication of films that are stable at neutral pH but that erode over a period of several days in acidic media (e.g., pH ∼5). Experiments using a structural analog of polymer >2 with carboxylate side chains that do not hydrolyze readily provided support for the view that the disruption of these films occurred as a result of polymer side chain hydrolysis and a resulting change in the net charge of the polymers. Because this approach is based upon the use of anionic polymers to induce film instability, it provides a platform for the design of multilayers that can be used to provide control over the release of cationic film components. As proof of concept, we demonstrated that ultrathin films ∼100 nm thick fabricated using polymer >2 sustain the release of fluorescently labeled PAH for up to four days when incubated at pH 5.0. The synthetic approach used here is modular and tunable and can be used to introduce anionic ‘charge-shifting’ character to a broad range of other polyamines. With further development, this approach could expand significantly the range of different cationic agents (e.g., cationic proteins, peptides, polymers, nanoparticles, etc.) that can be released or delivered from surfaces using polyelectrolyte multilayers.
机译：我们报告了一种“电荷转移”阴离子聚合物的设计方法，该方法可控制水性介质中超薄聚电解质多层的破坏。我们证明，将柠康酸酐添加到聚烯丙胺中会产生一种阴离子，羧酸盐官能化的聚合物（聚合物> 2 ），该聚合物在酸性环境中可以很容易地转换回阳离子聚烯丙胺。因此，将聚合物> 2 掺入聚电解质多层中提供了一种方法来制造在中性pH下稳定但在酸性介质（例如pH〜5）中腐蚀几天的薄膜。使用聚合物> 2 具有不水解的羧酸酯侧链的结构类似物进行的实验，为以下观点提供了支持，即这些膜的破坏是由于聚合物侧链水解而导致了膜的破坏。聚合物的净电荷。因为此方法基于使用阴离子聚合物引起薄膜不稳定性，所以它为多层设计提供了一个平台，该平台可用于控制阳离子薄膜成分的释放。作为概念验证，我们证明了使用聚合物> 2 制成的厚约100 nm的超薄薄膜在pH 5.0下孵育时，最多可持续四天释放荧光标记的PAH。此处使用的合成方法具有模块化和可调性，可用于将阴离子的“电荷转移”特性引入多种其他多胺中。随着进一步的发展，该方法可以显着扩展可以使用聚电解质多层从表面释放或递送的不同阳离子试剂（例如，阳离子蛋白，肽，聚合物，纳米颗粒等）的范围。

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