Stabilizing *<scp>OH</scp> intermediate by fabricating <scp>Ni₃N</scp>‐<scp>MoN</scp> for scalable 5‐hydroxymethylfurfural electrooxidation

Abstract Achieving large‐scale coupling of organic electrooxidation and the hydrogen evolution reaction, while understanding the competition between organic electrooxidation and oxygen evolution reaction (OER), is a significant challenge. In this study, using Ni 3 N‐MoN/NF, an efficient heterojunction electrocatalyst as both anode and cathode in a 50 cm 2 continuous flow reactor, we achieved a total current of ~20 A at 2.6 V. This resulted in the highest single‐pass 5‐hydroxymethylfurfural conversion efficiency (0.049 mmol cm −2 min −1 ) and gram‐level production of 2,5‐furandicarboxylic acid. Theoretical studies revealed that MoN accelerated *OH formation and increased its deprotonation energy barrier, leading to *OH accumulation, effectively promoting organic electrooxidation and inhibiting OER. We anticipate that our foundation in understanding the reaction mechanism and catalyst design strategy can be extended to a wider range of anodic oxidation reactions.