Coal-based Carbon Nanosheets Contained Carbon Microfibers Modified with Grown Carbon Nanotubes As Efficient Air Electrode Material for Rechargeable Zinc-Air Batteries

Coal-based oxygen electrocatalysts hold immense promise for cost-effective applications in rechargeable Zn-air batteries (ZABs) and the value-added, clean utilization of traditional coal resources. Herein, an electrospun membrane electrode comprising coal-derived carbon nanosheets and directly grown carbon nanotubes (CNS/ CMF@CNT) was successfully synthesized. The hierarchical porous structure of the electrode, composed of multiple components, significantly facilitates mass and ion transportation, resulting in exceptional electrochemical performance. Employing Fe as the catalyst for CNT growth, the CNS/CMF@CNT electrode exhibits a remarkable onset potential of 0.96 V and a half-wave potential of 0.87 V in the oxygen reduction reaction (ORR). In-situ surface-enhanced Raman spectroscopy reveals that hydroxyl radical desorption on the surface of CNS/ CMF@CNT(Fe) is the rate-determining step of the ORR. Notably, the aqueous ZAB featuring the CNS/CMF@CNT (Fe) electrode achieved a peak power density of 216.0 mW cm-2 at a current density of 414 mA cm-2 and maintained a voltage efficiency of 65.1 % after 2000 charge/discharge cycles at 5 mA cm-2. Furthermore, the allsolid-state ZAB incorporating this electrode displayed an open-circuit voltage of 1.43 V, a peak power density of 70.1 mW cm-2 at a current density of 110 mA cm-2, and a voltage efficiency of 66.5 % after 150 charge/ discharge cycles. The utilization of abundant coal as the raw material for electrode fabrication not only brings conceivable economic benefits in ZAB construction, but also commendably advances the effective application of traditional coal resources in a more sustainable manner.