Exploiting Antisite Defects in FeWN₂ Nanosheets for Enol Electro‐oxidation Coupled with H₂ Evolution at a Large Current Density

Hydrogen production from biomass electro-oxidation offers a promising alternative to water electrolysis by lowering the anodic oxidation barrier and producing valuable chemicals. However, current biomass electro-oxidation 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 antisite 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.