Anchoring Fe Species on the Highly Curved Surface of S and N Co‐Doped Carbonaceous Nanosprings for Oxygen Electrocatalysis and a Flexible Zinc‐Air Battery

Abstract Oxygen reduction reaction (ORR) is of critical significance in the advancement of fuel cells and zinc‐air batteries. The iron‐nitrogen (Fe−N x ) sites exhibited exceptional reactivity towards ORR. However, the task of designing and controlling the local structure of Fe species for high ORR activity and stability remains a challenge. Herein, we have achieved successful immobilization of Fe species onto the highly curved surface of S, N co‐doped carbonaceous nanosprings (denoted as FeNS/Fe 3 C@CNS). The induction of this twisted configuration within FeNS/Fe 3 C@CNS arose from the assembly of chiral templates. For electrocatalytic ORR tests, FeNS/Fe 3 C@CNS exhibits a half‐wave potential ( E 1/2 ) of 0.91 V in alkaline medium and a E 1/2 of 0.78 V in acidic medium. The Fe single atoms and Fe 3 C nanoparticles are coexistent and play as active centers within FeNS/Fe 3 C@CNS. The highly curved surface, coupled with S substitution in the coordination layer, served to reduce the energy barrier for ORR, thereby enhancing the intrinsic catalytic activity of the Fe single‐atom sites. We also assembled a wearable flexible Zn‐air battery using FeNS/Fe 3 C@CNS as electrocatalysts. This work provides new insights into the construction of highly curved surfaces within carbon materials, offering high electrocatalytic efficacy and remarkable performance for flexible energy conversion devices.