A Surface‐Oxide‐Rich Activation Layer (SOAL) on Ni2Mo3N for a Rapid and Durable Oxygen Evolution Reaction

The oxygen evolution reaction (OER) is key to renewable energy technologies such as water electrolysis and metal–air batteries. However, the multiple steps associated with proton‐coupled electron transfer result in sluggish OER kinetics and catalysts are required. Here we demonstrate that a novel nitride, Ni2Mo3N, is a highly active OER catalyst that outperforms the benchmark material RuO2. Ni2Mo3N exhibits a current density of 10 mA cm−2 at a nominal overpotential of 270 mV in 0.1 m KOH with outstanding catalytic cyclability and durability. Structural characterization and computational studies reveal that the excellent activity stems from the formation of a surface‐oxide‐rich activation layer (SOAL). Secondary Mo atoms on the surface act as electron pumps that stabilize oxygen‐containing species and facilitate the continuity of the reactions. This discovery will stimulate the further development of ternary nitrides with oxide surface layers as efficient OER catalysts for electrochemical energy devices. Ni2Mo3N performs excellently in the oxygen evolution reaction, outperforming the benchmark catalyst RuO2. This stems from a surface‐oxide‐rich activation layer (SOAL) where Ni atoms are the active sites and Mo atoms can be considered as an electron pump to transfer surface charges, stabilize the oxygen‐contained product species, and facilitate the continuity of the oxygen reactions.