Polymer-infiltrated nanoplatelet films with nacre-like structure via flow coating and capillary rise infiltration (CaRI)

Alignment of highly anisotropic nanomaterials in a polymer matrix can yield nanocomposites with unique mechanical and transport properties. Conventional methods of nanocomposite film fabrication are not well-suited for manufacturing composites with very high concentrations of anisotropic nanomaterials, potentially limiting the widespread implementation of these useful structures. In this work, we present a scalable approach to fabricate polymer-infiltrated nanoplatelet films (PINFs) based on flow coating and capillary rise infiltration (CaRI) and study the processing-structure-property relationship of these PINFs. We show that films with high aspect ratio (AR) gibbsite (Al (OH)3) nanoplatelets (NPTs) aligned parallel to the substrate can be prepared using a flow coating process. NPTs are highly aligned with a Herman's order parameter of 0.96 and a high packing fraction >80 vol%. Such packings show significantly higher fracture toughness compared to low AR nanoparticle (NP) packings. By depositing NPTs on a polymer film and subsequently annealing the bilayer above the glass transition temperature of the polymer, polymer infiltrates into the tortuous NPT packings though capillarity. We observe larger enhancement in the modulus, hardness and scratch resistance of NPT films upon polymer infiltration compared to NP packings. The excellent mechanical properties of such films benefit from both thermally promoted oxide bridge formation between NPTs as well as polymer infiltration increasing the strength of NPT contacts. Our approach is widely applicable to highly anisotropic nanomaterials and allows the generation of mechanically robust polymer nanocomposite films for a diverse set of applications.