Double-Holey-Heterostructure Frameworks Enable Fast, Stable, and Simultaneous Ultrahigh Gravimetric, Areal, and...

Deliberate design of advantageous nanostructures holds great promise for developing high-performance electrode materials for electrochemical energy storage. However, it remains a tremendous challenge to simultaneously gain high gravimetric, areal, and volumetric capacities as well as high rate performance and cyclability to meet practical requirements mainly due to the intractable insufficient ion diffusion and limited active sites for dense electrodes with high areal mass loadings. Herein we report a double-holey-heterostructure framework, in which holey Fe₂O₃ nanosheets (H-Fe₂O₃) are tightly and conformably grown on the holey reduced graphene oxide (H-RGO). This hierarchical nanostructure allows for rapid ion and electron transport and sufficient utilization of active sites throughout a highly compact and thick electrode. Therefore, the free-standing flexible H-Fe₂O₃/H-RGO heterostructure anode can simultaneously deliver ultrahigh gravimetric, areal, and volumetric capacities of 1524 mAh g^-1, 4.72 mAh cm^-2, and 2621 mAh cm^-3, respectively, at 0.2 A g^-1 after 120 cycles, and extraordinary rate performance with a capacity of 487 mAh g^-1 (1.51 mAh cm^-2) at a high current density of 30 A g^-1 (93 mA cm^-2) as well as excellent cycling stability with a capacity retention of 96.3% after 1600 cycles, which has rarely been achieved before.