CuCo2S4 Nanosheets@N‐Doped Carbon Nanofibers by Sulfurization at Room Temperature as Bifunctional Electrocatalysts in Flexible Quasi‐Solid‐State Zn–Air Batteries

The performance of quasi-solid-state flexible zinc-air batteries (ZABs) is critically dependent on the advancement of air electrodes with outstanding bifunctional electrocatalysis for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), together with the desired mechanical flexibility and robustness. The currently available synthesis processes for high-efficiency bifunctional bimetallic sulfide electrodes typically require high-temperature hydrothermal or chemical vapor deposition, which is undesirable in terms of the complexity in experimental procedure and the damage of flexibility in the resultant electrode. Herein, a scalable fabrication process is reported by combining electrospinning with in situ sulfurization at room temperature to successfully obtain CuCo2S4 nanosheets@N-doped carbon nanofiber (CuCo2S4 NSs@N-CNFs) films, which show remarkable bifunctional catalytic performance (Ej= 10 (OER) - E1/2 (ORR) = 0.751 V) with excellent mechanical flexibility. Furthermore, the CuCo2S4 NSs@N-CNFs cathode delivers a high open-circuit potential of 1.46 V, an outstanding specific capacity of 896 mA h g-1, when assembled into a quasi-solid-state flexible ZAB together with Zn NSs@carbon nanotubes (CNTs) film (electrodeposited Zn nanosheets on CNTs film) as the anode. The ZAB also shows a good flexibility and capacity stability with 93.62% capacity retention (bending 1000 cycles from 0° to 180°), making it an excellent power source for portable and wearable electronic devices.