LAUSR

Despite recent progress in the synthesis and application of graphene-based aerogels, some challenges such as scalable and cost-effective production, and miniaturization still remain, which hinder the practical application of these materials. Here we report a large-scale electrospinning method to generate graphene-based aerogel microspheres (AMs), which show broadband, tunable and high-performance microwave absorption. Graphene/Fe3O4 AMs with a large number of openings with hierarchical connecting radial microchannels can be obtained via electrospinning-freeze drying followed by calcination. Importantly, for a given Fe3O4:graphene mass ratio, altering the shape of aerogel monoliths or powders into aerogel microspheres leads to unique electromagnetic wave properties. As expected, the reflection loss of graphene/Fe3O4 AMs-1:1 with only 5 wt.% absorber loading reaches −51.5 dB at 9.2 GHz with a thickness of 4.0 mm and a broad absorption bandwidth (RL < −10 dB) of 6.5 GHz. Furthermore, switching to coaxial electrospinning enables the fabrication of SiO2 coatings to construct graphene/Fe3O4@SiO2 core‒shell AMs. The coatings influence the electromagnetic wave absorption of graphene/Fe3O4 AMs significantly. In view of these advantages, we believe that this processing technique may be extended to fabricate a wide range of unique graphene-based architectures for functional design and applications.