Ultralight Three-Dimensional Hierarchical Cobalt Nanocrystals/N-Doped CNTs/Carbon Sponge Composites with a Hollow Skeleton toward Superior Microwave Absorption.

It is extremely desirable but remains greatly challenging to obtain high-performance microwave absorption (MA) materials with thin thickness, lightweight, wide frequency bandwidth, and strong absorption by facile and low-cost preparing methods. In this work, by utilizing an inexpensively commercial melamine-formaldehyde sponge (MFS) as a template for growth of a Co-based metal-organic framework (ZIF-67) and subsequently carbonizing this ZIF-67-decorated MFS in a nitrogen atmosphere, an ultralight (8 mg cm-3), three-dimensional hybrid carbon sponge composite with a hierarchical micro/nanostructure and hollow skeleton is successfully prepared to acquire excellent MA performances for the first time. The as-obtained composite consisted of interconnected carbon microtubes as a skeleton, intertwined N-doped carbon nanotubes (CNTs) grew on the outer surface of the carbon microtubes, and metallic Co nanocrystals encapsulated at the tips of the CNTs. Benefiting from the unique architecture and hierarchical composite which contribute to a good conductive network, moderate magnetic loss, strong matched impedance, and multiple polarization, the composite (Co/CNTs/CS) exhibited a minimum reflection loss (RL) of -51.2 dB and an effective absorption bandwidth (EAB, RL < -10 dB) of 4.1 GHz with a matching thickness of 2.2 mm at a filler loading of as low as 10 wt % in paraffin wax. Even with the thickness of 1.6 mm or at the filler loading of 5 wt %, the composites can also gain the low minimum RL value of -30.9 or -17.9 dB, respectively. In addition, the largest EAB was 5.4 GHz at the thickness of 2.0 mm, and the tunable EAB can be achieved in the range of 3.6-18 GHz, covering 90% of the measured frequency range via adjusting the absorber thickness between 1 and 5.5 mm. The results offer new insights for designing advanced microwave absorbers with lightweight, thin thickness, strong RL, and wide absorption frequency range.