不互溶液界面氢键作用下polymer膜的生长机理
Growth mechanism of polymer membranes obtained by H-bonding across immiscible liquid interfaces
摘要：
聚合物在液体界面处的络合是一种新兴的技术，用于生产全液体可印刷和自修复装置和膜。控制组装过程至关重要，但起作用的机制仍不清楚。采用两种不同的反射率测量方法，研究了氢键PPO-PMAA膜在平坦液-液界面上的自发生长。我们发现，膜厚度h随时间t的增长为h~t^（1/2），这是一个扩散限制的过程。然而，与直觉相反，我们观察到随着PPO摩尔质量的增加，该过程更快。我们能够合理化这些结果与模型，认为PPO链的扩散内生长的膜。后者的架构被描述为凝胶状多孔网络，具有比扩散PPO链的半径小得多的孔径，从而诱导阻碍扩散过程的熵屏障。从实验数据和模型结果之间的比较中，我们提取了一些关于膜的微观结构的关键信息。该研究为合理设计具有最佳性能的自组装膜和胶囊开辟了道路。
英文摘要：
Complexation of polymers at liquid interfaces is an emerging technique to produce all-liquid printable and self-healing devices and membranes. It is crucial to control the assembly process but the mechanisms at play remain unclear. Using two different reflectometric methods, we investigate the spontaneous growth of H-bonded PPO-PMAA membranes at a flat liquid-liquid interface. We find that the membrane thickness h grows with time t as h~t^(1/2), which is reminiscent of a diffusion-limited process. However, counter-intuitively, we observe that this process is faster as the PPO molar mass increases. We are able to rationalize these results with a model which considers the diffusion of the PPO chains within the growing membrane. The architecture of the latter is described as a gel-like porous network, with a pore size much smaller than the radius of the diffusing PPO chains, thus inducing entropic barriers that hinder the diffusion process. From the comparison between the experimental data and the result of the model, we extract some key piece of information about the microscopic structure of the membrane. This study opens the route toward the rational design of self-assembled membranes and capsules with optimal properties.
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