Exploiting Anti‐site Defects in FeWN2 Nanosheets for Enol Electrooxidation Coupled with H2 Evolution at a Large Current Density

Hydrogen production from biomass electrooxidation offers a promising alternative to water electrolysis by lowering the anodic oxidation barrier and producing valuable chemicals. However, current biomass electrooxidation systems have difficulties in achieving an industrial‐scale current density due to the difficulty in cleaving high‐energy C‐H and O‐H bonds. Here, we report a ternary layer nitride FeWN2 electrocatalyst with abundant anti‐site defects (ASDs), which significantly improves its electrocatalytic performance for ascorbic acid (AA) oxidation. The catalyst works at a remarkable current density of 2.5 A cm‐2 at 0.69 V (vs. RHE) and achieves 4 A cm‐2 at 1.12 V in a two‐electrode electrolyzer at 60°C with 100% Faraday efficiency for H2 production. Theoretical calculations reveal that W atoms near antipodal Fe sites replenish the electron density of Fe, maintaining moderate Fe‐DHA adsorption strength induced by ASDs that achieve superior catalytic efficiency for AA‐to‐DHA conversion This study provides new insight for developing high‐performance organic oxidation catalysts with ASDs.