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  1. Abstract

    Despite being a pillar of high‐performance materials in industry, manufacturing carbon fiber composites with simultaneously enhanced multifunctionality and structural properties has remained elusive due to the lack of practical bottom‐up approaches with control over nanoscale interactions. Guided by the droplet's internal currents and amphiphilicity of nanomaterials, herein, a programmable spray coating is introduced for the deposition of multiple nanomaterials with tailorable patterns in composite.  It is shown that such patterns regulate the formation of interfaces, damage containment, and electrical‐thermal conductivity of the composites, which is absent in conventional manufacturing that primarily rely on incorporating nanomaterials to achieve specific functionalities. Molecular dynamics simulations show that increasing the hydrophilicity of the hybrid nanomaterials, which is synchronous with shifting patterns from disk to ring, improves the interactions between the carbon surfaces and epoxy at the interfaces,manifested in enhanced interlaminar and flexural performance. Transitioning from ring to disk creates a larger interconnected network  leading to improved thermal and electrical properties without penalty in mechanical properties. This novel approach introduces a new design , where the mechanical and multifunctional performance is controlled by the shape of the deposited patterns, thus eliminating the trade‐off between properties that are considered paradoxical in today's manufacturing of hierarchical composites.

     
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  2. Abstract

    Achieving desired performance from self‐assembly of nanoparticles (NPs) is challenging due to the stochastic nature of interactions among the constituent building blocks. Self‐assembly of nano‐colloids through evaporation of particle‐laden droplets can be exploited to fabricate tailored nanostructures that add functionality and engineer the properties of manufactured components. The particle–particle and particle–solvent interactions, and delicate force balance among them are the main factors that define the pattern of the final 3D nanostructure. Here, a nanoparticle‐agnostic approach that allows the fabrication of nanostructures with precisely engineered patterns is introduced. Evaporative droplets of aqueous suspensions of pristine Carbon Nanotubes, Graphene Nanoplatelets, and Boron Nitride Nanotubes representing NPs of different elemental compositions, sizes, and shapes are investigated. Cellulose nanocrystals (CNCs) are used as a platform to make hybrid systems of CNC‐NP and utilize the repulsive‐attractive‐directional interactions in these multimaterial systems to enforce the desired final pattern between ring and disk. It is shown that irrespective of the type of NPs, the amphiphilicity of the hybrid system dictates the formation of deposited patterns. Finally, the effect of self‐assembled patterns on the functionality of multi‐material systems is demonstrated. The proposed method creates new capabilities in the precisely controlled nanostructures and facilitates smart self‐assembly systems.

     
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  3. Free, publicly-accessible full text available June 1, 2025