Single‐atom catalysts (SACs) are attracting widespread interest for the catalytic oxygen reduction reaction (ORR), with Fe−Nx SACs exhibiting the most promising activity. However, Fe‐based catalysts suffer serious stability issues as a result of oxidative corrosion through the Fenton reaction. Herein, using a metal‐organic framework as an anchoring matrix, we for the first time obtained pyrolyzed Cr/N/C SACs for the ORR, where the atomically dispersed Cr is confirmed to have a Cr−N4 coordination structure. The Cr/N/C catalyst exhibits excellent ORR activity with an optimal half‐wave potential of 0.773 V versus RHE. More excitingly, the Fenton reaction is substantially reduced and, thus, the final catalysts show superb stability. The innovative and robust active site for the ORR opens a new possibility to circumvent the stability issue of the non‐noble metal ORR catalysts.

Fuel cell, a sustainable technology that assures a cleaner earth, once experienced disillusion due to the issue of economic viability associated with the massive usage of Pt-based catalysts. To address...