约束对Polymer（SIP）在纳米填料中溶剂驱动渗透的影响
Effect of Confinement on Solvent-driven Infiltration of Polymer (SIP) into Nanoparticle Packings
摘要：
在聚合物基体中含有高体积分数（> 50vol%）的纳米颗粒（NP）的纳米复合膜具有作为结构涂层的功能和用途的前景，并且还提供了理解强约束下的聚合物行为的独特平台。在此之前，我们开发了一种新的技术，在室温下使用溶剂驱动的聚合物（SIP）渗透到NP包装制造这样的纳米复合材料。在SIP工艺中，由下面的聚合物膜和NP的致密填料制成的双层暴露于溶剂蒸气，这引起溶剂冷凝到填料的空隙中。冷凝的溶剂塑化下面的聚合物膜，诱导聚合物渗透到NP填料中的溶剂填充的空隙中。在这项工作中，我们研究了限制SIP的动力学和最终分配的NP填料的间隙的聚合物的效果。我们发现，虽然在SIP渗透的动态是强烈依赖于禁闭，渗透的最终程度是独立的禁闭。渗透的时间服从幂律约束，如由链尺寸和孔径的比率定义的。定性地说，所观察到的时间尺度是由于浓度制度的变化，渗透的进行，这导致随着时间的推移，在系统中的特征长度尺度的变化。当孔中的浓度超过临界重叠浓度时，聚合物的特征长度尺度不再是整个链的特征长度尺度，而是小于孔径的相关长度。因此，在很长一段时间，渗透的程度是独立的约束比。此外，聚合物和纳米颗粒之间有利的表面相互作用增强了分配到NP填料中。
英文摘要：
Nanocomposite films containing a high volume fraction (> 50vol%) of nanoparticles (NPs) in a polymer matrix are promising for their functionality and use as structural coatings, and also provide a unique platform to understand polymer behavior under strong confinement. Previously, we developed a novel technique to fabricate such nanocomposites at room temperature using solvent-driven infiltration of polymer (SIP) into NP packings. In the SIP process, a bilayer made of an underlying polymer film and a dense packing of NPs is exposed to solvent vapor which induces condensation of the solvent into the voids of the packing. The condensed solvent plasticizes the underlying polymer film, inducing polymer infiltration into the solvent-filled voids in the NP packing. In this work, we study the effect of confinement on the kinetics of SIP and the final partitioning of polymer into the interstices of the NP packing. We find that, while the dynamics of infiltration during SIP are strongly dependent on confinement, the final extent of infiltration is independent of confinement. The time for infiltration obeys a power law with confinement, as defined by the ratio of the chain size and the pore size. Qualitatively, the observed time scale is attributed to changes in concentration regimes as infiltration proceeds, which lead to shifting characteristic length scales in the system over time. When the concentration in the pore exceeds the critical overlap concentration, the characteristic length scale of the polymer is no longer that of the entire chain, but rather the correlation length, which is smaller than the pore size. Therefore, at long times, the extent of infiltration is independent of the confinement ratio. Furthermore, favorable surface interactions between the polymer and the nanoparticles enhance partitioning into the NP packing.
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