Nanoporous Polymer-Infiltrated Nanoparticle Films with Uniform or Graded Porosity via Undersaturated Capillary Rise Infiltration.
Nanoporous Polymer-Infiltrated Nanoparticle Films with Uniform or Graded Porosity via Undersaturated Capillary Rise Infiltration.
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DOI：
10.1021/acsnano.7b00298
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发表时间：
2017-02
期刊：
影响因子：
17.1
通讯作者：
Jyo Lyn Hor;Yijie Jiang;D. Ring;Robert A. Riggleman;K. Turner;Daeyeon Lee
中科院分区：
文献类型：
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作者：
Jyo Lyn Hor;Yijie Jiang;D. Ring;Robert A. Riggleman;K. Turner;Daeyeon Lee
在这项工作中，我们提出了制造纳米多孔聚合物渗透纳米粒子薄膜（PINFs）的基础上不饱和毛细上升渗透（UCaRI）的均匀或梯度孔隙率，并研究这些纳米多孔PINFs的工艺-结构-性能的关系。UCaRI方法涉及首先在聚合物层顶上产生随机填充的纳米颗粒层的双层膜，使得聚合物的体积小于纳米颗粒填充中的空隙体积。随后，双层膜在高于聚合物的玻璃化转变温度下退火，以诱导聚合物渗透到纳米颗粒填料的空隙中。使用原位光谱椭圆偏振和分子动力学模拟，我们观察到，聚合物的运输发生在两个阶段：毛细作用引起的渗透，然后逐渐蔓延，可能通过表面扩散。通过改变退火时间，UCaRI能够生成分级或均匀的纳米多孔PINF。我们还表明，这些纳米多孔PINFs具有可调的光学和机械性能，这可以简单地通过改变初始双层中的纳米颗粒与聚合物层的厚度比来定制。UCaRI方法是通用的，广泛适用于各种聚合物，这允许生成用于多种应用的纳米多孔PINF。
In this work, we present the fabrication of nanoporous polymer-infiltrated nanoparticle films (PINFs) with either uniform or graded porosity based on undersaturated capillary rise infiltration (UCaRI) and study the processing-structure-property relationship of these nanoporous PINFs. The UCaRI process involves first generating a bilayer film of a randomly packed nanoparticle layer atop a polymer layer, such that the volume of the polymer is less than the void volume in the nanoparticle packing. Subsequently, the bilayer film is annealed above the glass transition temperature of the polymer to induce polymer infiltration into the voids of the nanoparticle packing. Using in situ spectroscopic ellipsometry and molecular dynamics simulations, we observe that the polymer transport occurs in two stages: capillarity-induced infiltration, followed by gradual spreading, likely via surface diffusion. By varying the annealing time, UCaRI enables the generation of graded or uniform nanoporous PINFs. We also show that these nanoporous PINFs have tunable optical and mechanical properties, which can be tailored simply by changing the nanoparticle to polymer layer thickness ratio in the initial bilayer. The UCaRI approach is versatile and widely applicable to various polymers, which allows generation of nanoporous PINFs for multiple applications.