Structural Color from Cellulose Nanocrystals or Chitin Nanocrystals: Self-Assembly, Optics, and Applications.

Widespread concerns over the impact of human activity on the environment have resulted in a desire to replace artificial functional materials with naturally derived alternatives. As such, polysaccharides are drawing increasing attention due to offering a renewable, biodegradable, and biocompatible feedstock for functional nanomaterials. In particular, nanocrystals of cellulose and chitin have emerged as versatile and sustainable building blocks for diverse applications, ranging from mechanical reinforcement to structural coloration. Much of this interest arises from the tendency of these colloidally stable nanoparticles to self-organize in water into a lyotropic cholesteric liquid crystal, which can be readily manipulated in terms of its periodicity, structure, and geometry. Importantly, this helicoidal ordering can be retained into the solid-state, offering an accessible route to complex nanostructured films, coatings, and particles. In this review, the process of forming iridescent, structurally colored films from suspensions of cellulose nanocrystals (CNCs) is summarized and the mechanisms underlying the chemical and physical phenomena at each stage in the process explored. Analogy is then drawn with chitin nanocrystals (ChNCs), allowing for key differences to be critically assessed and strategies toward structural coloration to be presented. Importantly, the progress toward translating this technology from academia to industry is summarized, with unresolved scientific and technical questions put forward as challenges to the community.

Large-scale fabrication of structurally coloured cellulose nanocrystal films and effect pigments.

Cellulose nanocrystals are renewable plant-based colloidal particles capable of forming photonic films by solvent-evaporation-driven self-assembly. So far, the cellulose nanocrystal self-assembly process has been studied only at a small scale, neglecting the limitations and challenges posed by the continuous deposition processes that are required to exploit this sustainable material in an industrial context. Here, we addressed these limitations by using roll-to-roll deposition to produce large-area photonic films, which required optimization of the formulation of the cellulose nanocrystal suspension and the deposition and drying conditions. Furthermore, we showed how metre-long structurally coloured films can be processed into effect pigments and glitters that are dispersible, even in water-based formulations. These promising effect pigments are an industrially relevant cellulose-based alternative to current products that are either micro-polluting (for example, non-biodegradable microplastic glitters) or based on carcinogenic, unsustainable or unethically sourced compounds (for example, titania or mica).

Structurally Colored Radiative Cooling Cellulosic Films.

Daytime radiative cooling (DRC) materials offer a sustainable approach to thermal management by exploiting net positive heat transfer to deep space. While such materials typically have a white or mirror-like appearance to maximize solar reflection, extending the palette of available colors is required to promote their real-world utilization. However, the incorporation of conventional absorption-based colorants inevitably leads to solar heating, which counteracts any radiative cooling effect. In this work, efficient sub-ambient DRC (Day: -4 °C, Night: -11 °C) from a vibrant, structurally colored film prepared from naturally derived cellulose nanocrystals (CNCs), is instead demonstrated. Arising from the underlying photonic nanostructure, the film selectively reflects visible light resulting in intense, fade-resistant coloration, while maintaining a low solar absorption (≈3%). Additionally, a high emission within the mid-infrared atmospheric window (>90%) allows for significant radiative heat loss. By coating such CNC films onto a highly scattering, porous ethylcellulose (EC) base layer, any sunlight that penetrates the CNC layer is backscattered by the EC layer below, achieving broadband solar reflection and vibrant structural color simultaneously. Finally, scalable manufacturing using a commercially relevant roll-to-roll process validates the potential to produce such colored radiative cooling materials at a large scale from a low-cost and sustainable feedstock.