Polynary transition‐metal atom catalysts are promising to supersede platinum (Pt)‐based catalysts for oxygen reduction reaction (ORR). Regulating the local configuration of atomic catalysts is the key to catalyst performance enhancement. Different from the previously reported single‐atom or dual‐atom configurations, a new type of ternary‐atom catalyst, which consists of atomically dispersed, nitrogen‐coordinated Co–Co dimers, and Fe single sites (i.e., Co2–N6 and Fe–N4 structures) that are coanchored on highly graphitized carbon supports is developed. This unique atomic ORR catalyst outperforms the catalysts with only Co2–N6 or Fe–N4 sites in both alkaline and acid conditions. Density functional theory calculations clearly unravels the synergistic effect of the Co2–N6 and Fe–N4 sites, which can induce higher filling degree of Fe–d orbitals and favors the binding capability to *OH intermediates (the rate determining step). This ternary‐atom catalyst may be a promising alternative to Pt to drive the cathodic ORR in zinc–air batteries.

Ultra-thin N-doped-graphene encapsulated Ni nanoparticles coupled with MoO2 nanosheets are prepared for HER and OER. As used for overall water splitting, it can work for 196 h at 1000 mA cm−2.

Through the modification of the surface and bulk electronic structures of Ru, the developed Ru-based catalyst presents superior electrocatalytic hydrogen and oxygen evolution activities with great durability over a wide pH range.