In Situ Activating Strategy to Significantly Boost Oxygen Electrocatalysis of Commercial Carbon Cloth for Flexible and Rechargeable Zn‐Air Batteries

An in situ strategy to simultaneously boost oxygen reduction and oxygen evolution (ORR/OER) activities of commercial carbon textiles is reported and the direct use of such ubiquitous raw material as low‐cost, efficient, robust, self‐supporting, and bifunctional air electrodes in rechargeable Zn‐air batteries is demonstrated. This strategy not only furnishes carbon textiles with a large surface area and hierarchical meso‐microporosity, but also enables efficient dual‐doping of N and S into carbon skeletons while retaining high conductivity and stable monolithic structures. Thus, although original carbon textile has rather poor catalytic activity, the activated textiles without loading other active materials yield effective ORR/OER bifunctionality and stability with a much lower reversible overpotential (0.87 V) than those of Pt/C (1.10 V) and RuO(2) (1.02 V) and many reported metal‐free bifunctional catalysts. Importantly, they can concurrently function as current collectors and as ORR/OER catalysts for rechargeable aqueous and flexible solid‐state Zn‐air batteries, showing excellent cell performance, long lifetime, and high flexibility.