Single-atom catalysts with high activity and efficient atom utilization have great potential in the electrocatalysis field, especially for rechargeable zinc-air batteries (ZABs). However, it is still a serious challenge to rationally construct a single-atom catalyst with satisfactory electrocatalytic activity and long-term stability. Here, we simultaneously realize the atomic-level dispersion of cobalt and the construction of carbon nanotube (CNT)-linked N-doped porous carbon nanofibers (NCFs) via an electrospinning strategy. In this hierarchical structure, the Co-N4 sites provide efficient oxygen reduction/evolution electrocatalytic activity, the porous architectures of NCFs guarantee the active site's accessibility, and the interior CNTs enhance the flexibility and mechanical strength of porous fibers. As a binder-free air cathode, the as-prepared catalysts deliver superdurability of 600 h at 10 mA cm-2 for aqueous ZABs and considerable flexibility and a small voltage gap for all-solid-state ZABs. This work provides an effective single-atom design/nanoengineering for superdurable zinc-air batteries.
Keywords: bifunctional oxygen electrocatalysis; electrospinning; flexible carbon membranes; rechargeable Zn−air batteries; single-atom catalysts.