No abstract

Achieving a structural hierarchy and a uniform nanofiller dispersion simultaneously remains highly challenging for obtaining a robust polymer nanocomposite of immiscible components. In this study, a remarkably facile Pickering emulsification approach is developed to fabricate hierarchical composites of immiscible acrylic polymer and native cellulose nanofibers by taking advantage of the dual role of the nanofibers as both emulsion stabilizer and polymer reinforcement. The composites feature a unique "reverse" nacre-like microstructure reinforced with a well-dispersed two-tier hierarchical nanofiber network, leading to a synergistic high strength, modulus, and toughness (20, 50, and 53 times that of neat polymer, respectively), high optical transparency (89%), high flexibility, and a drastically low thermal expansion (13 ppm K, 1/15th of the neat polymer). The nanocomposites have a three-dimensional-shape moldability, also their surface can be patterned with micro/nanoscale features with high fidelity by in situ compression molding, making them attractive as the substrate for flexible displays, smart contact lens devices, and photovoltaics. The Pickering emulsification approach should be broadly applicable for the fabrication of novel functional materials of various immiscible components.

A low thermally expanded transparent film is developed by exploiting wood fibers that can be considered to be nanostructured fibers in which individual nanofibers do not significantly agglomerate and are oriented parallel to the fiber direction. It is thereby demonstrated that paper, used since ancient times, will be a next‐generation optical material.

The recent rapid expansion of thin-film, bendable, and wearable consumer (opto)­electronics demands flexible and transparent substrates other than glass. Plastics are the traditional choice, but they require amelioration because of their thermal instability. Here, we report the successful conversion of a soft and thermally vulnerable polymer into a highly thermally stable transparent nanocomposite material. This is achieved by the meticulous choice of a polymer with a glass-transition temperature below 0 °C that gives stable mechanics above room temperature, reinforcing the polymer with a load-bearing hierarchical network of the incredibly strong and stable natural material: cellulose nanorods. Owing to the Pickering emulsification process, the nanocomposites inherit the self-assembled structural hierarchy from the cellulose nanorod-encapsulated resin droplets. The ameliorated nanocomposites have highly desirable high-temperature endurance (∼150–180 °C) in terms of the thermomechanical, thermodimensional, and thermo-optical performance. Any photonic nano- or microstructures can be directly molded on the surface of the nanocomposites in high precision for better light management in photonic and opto-electronic applications. The highlight of this work is the demonstration of a highly thermally stable microlens array on the ameliorated transparent nanocomposite.