Graphene aerogel has attracted great attention due to its unique properties, such as ultralow density, superelasticity, and high specific surface area. It shows huge potential in energy devices, high-performance pressure sensors, contaminates adsorbents, and electromagnetic wave absorbing materials. However, there still remain some challenges to further promote the development and real application of graphene aerogel including cost-effective scalable fabrication and miniaturization with group effect. This study shows millimeter-scale superelastic graphene aerogel spheres (GSs) with group effect and multifunctionality. The GSs are continuously fabricated on a large scale by wet spinning of graphene oxide liquid crystals followed by facile drying and thermal annealing. Such GS has an unusual core-shell structure with excellent elasticity and specific strength. Significantly, both horizontally and vertically grouped spheres exhibit superelasticity comparable to individual spheres, enabling it to fully recover at 95% strain, and even after 1000 compressive cycles at 70% strain, paving the way to wide applications such as pressure-elastic and adsorbing materials. The GS shows a press-fly behavior with an extremely high jump velocity up to 1.2 m s . For the first time, both free and oil-adsorbed GSs are remotely manipulated on water by electrostatic charge due to their ultralow density and hydrophobic properties.

Graphene flake size has a profound effect on the mechanical performance of the assembled graphene aerogels, particularly their strength, modulus and fatigue resistance under compression.

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The layer-by-layer (LbL) assembly approach has been widely used to fabricate multilayer coatings on substrates with multiple cycles, whereas it is hard to access thick films efficiently. Here, we developed an ion diffusion-directed assembly (IDDA) strategy to rapidly make multilayer thick coatings in one step on arbitrary substrates. To achieve multifunctional coatings, graphene oxide (GO) and metallic ions were selected as the typical building blocks and diffusion director in IDDA, respectively. With diffusion of metallic ions from substrate to negatively charged GO dispersion spontaneously (i.e., from high-concentration region to low-concentration region), GO was assembled onto the substrate sheet-by-sheet via sol-gel transformation. Because metallic ions with size of subnanometers can diffuse directionally and freely in the aqueous dispersion, GO was coated on the substrate efficiently, giving rise to films with desired thickness up to 10 μm per cycle. The IDDA approach shows three main merits: (1) high efficiency with a μm-scale coating rate; (2) controllability over thickness and evenness; and (3) generality for substrates of plastics, metals and ceramics with any shapes and morphologies. With these merits, IDDA strategy was utilized in the efficient fabrication of functional graphene coatings that exhibit outstanding performance as supercapacitors, electromagnetic interference shielding textiles, and anticorrosion coatings. This IDDA approach can be extended to other building blocks including polymers and colloidal nanoparticles, promising for the scalable production and application of multifunctional coatings.

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