Bimetallic Metal–Organic Framework-Derived Pomegranate-like Nanoclusters Coupled with CoNi-Doped Graphene for Strong Wideband Microwave Absorption

Metal–organic frameworks (MOFs) featuring high porosity and tunable structure make them become promising candidates to fabricate carbon-based microwave absorption (MA) materials to meet the requirements of electronic reliability and defense security. However, it is challenging to rationally design a well-organized micro-nanostructure to simultaneously achieve strong and wideband MA performance. Herein, a three-dimensional (3D) hierarchical nanoarchitecture (CoNi@NC/rGO-600) comprising pomegranate-like CoNi@NC nanoclusters and ultrasmall CoNi-decorated graphene has been successfully fabricated to broaden the absorption bandwidth and enhance the absorption intensity. The results confirm that the bimetallic MOF CoNi-BTC-derived pomegranate-like CoNi@NC nanoclusters with porous carbon shell as “peel” and sub-5 nm CoNi nanoparticles as “seeds” favor multiple polarization, magnetic loss, and impedance matching. Moreover, the interconnected 3D CoNi-doped graphene acts not only as a bridge to connect pomegranate-like CoNi@NC nanoclusters but also as a conductive network to supply multiple electron transportation paths. Consequently, the optimized CoNi@NC/rGO-600 exhibits extraordinary MA performance in terms of wide bandwidth (6.7 GHz) and strong absorption (−68.0 dB). As an effective strategy, this work provides a new insight into fabricating hierarchical composite structures for advancing MA performances and other applications.