Stabilizing *OH intermediate by fabricating Ni3N‐MoN 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.