Atomic interface engineering is an effective pathway to regulate the performance of single metal atom catalysts for electrochemical reactions in energy applications. Herein, we construct a sulfur modified Mn–N–C single atom catalyst through a metal–organic framework derived atomic interface strategy, which exhibits outstanding ORR activity with a half-wave potential of 0.916 V vs. RHE in alkaline media. Moreover, operando X-ray absorption spectroscopy analysis indicates that the isolated bond-length extending the low-valence Mn–N4–CxSy moiety serves as an active site during the ORR process. These findings suggest a promising method for the advancement of single atom catalysis.
