Nature‐inspired N, O Co‐Coordinated Manganese Single‐Atom Catalyst for Efficient Hydrogen Peroxide Electrosynthesis

Abstract The two‐electron oxygen reduction reaction (2e − ORR) is a pivotal pathway for the distributed production of hydrogen peroxide (H 2 O 2 ). In nature, enzymes containing manganese (Mn) centers can convert reactive oxygen species into H 2 O 2 . However, Mn‐based heterogeneous catalysts for 2e − ORR are scarcely reported. Herein, we developed a nature‐inspired single‐atom electrocatalyst comprising N, O co‐coordinated Mn sites, utilizing carbon dots as the modulation platform (Mn CD/C). As‐synthesized Mn CD/C exhibited exceptional 2e − ORR activity with an onset potential of 0.786 V and a maximum H 2 O 2 selectivity of 95.8 %. Impressively, Mn CD/C continuously produced 0.1 M H 2 O 2 solution at 200 mA/cm 2 for 50 h in the flow cell, with negligible loss in activity and H 2 O 2 faradaic efficiency, demonstrating practical application potential. The enhanced activity was attributed to the incorporation of Mn atomic sites into the carbon dots. Theoretical calculations revealed that the N, O co‐coordinated structure, combined with abundant oxygen‐containing functional groups on the carbon dots, optimized the binding strength of intermediate *OOH at the Mn sites to the apex of the catalytic activity volcano. This work illustrates that carbon dots can serve as a versatile platform for modulating the microenvironment of single‐atom catalysts and for the rational design of nature‐inspired catalysts.