• Energy Research
• 2021-2025close

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AbstractDaytime 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.

To meet the increasing demand for sustainable products, one can look to nature to scout new functional materials. For instance, the most brilliant and striking colours in plants are obtained using cellulose nanofibrils organised in helicoidal architectures. Interestingly, similar helicoidal architectures with analogous optical response can be obtained in vitro by self-assembly of cellulose nanocrystals (CNCs). CNCs are rod-like colloids capable of arranging into a liquid crystalline phase above a critical concentration in suspension. So far, the process that governs the self-assembly of CNCs into photonic structures was studied only at small scale. This neglects the limitations and challenges posed by large-scale and continuous processes which are prevalent in industrial contexts. In this thesis, I demonstrate how the self-assembly of CNCs can be precisely controlled to produce meters-long films using a roll-to-roll (R2R) equipment. Starting with commercially available material, the preparation of CNC suspension was optimised for R2R deposition to produce films with vibrant photonic colour across the visible range. Particularly, I discuss how the suspension properties, the casting parameters and drying time relate to the optical properties of the produced films. To validate the use of such materials for pigment preparation, I develop a protocol to produce a series of coloured microparticles from R2R-cast CNC films. The optical properties of the CNC microparticles were then assessed in various environment and finally benchmarked against other commercial effect pigments and glitters.