Convergent Valorization via Scalable C═N Bond Electrosynthesis Through Metal‐Dopant Interfacial Engineering in a Flow Electrolyzer

Abstract

ABSTRACT Electrocatalytic conversion of C‐ and N‐containing pollutants into value‐added C–N‐bond containing compounds has attracted increasing attention. Specifically, the exploration centers on the generation of oximes featuring C═N bonds, which are essential chemicals with widespread applications in the pharmaceutical and fine chemical fields. Here, we develop an integrated electrocatalytic platform to produce formaldoxime as the target product in a green solvent using metal‐doped MoS 2 as efficient catalysts. Notably, Fe‐doped MoS 2 significantly boosts the Faradaic efficiency and yield rate for H 2 C═NOH to 81.2% and 963 mmol h −1  g −1 , respectively. Mechanistic studies reveal that the Fe dopants enhance the NO 2 – bonding, promoting substrate engagement and subsequently H 2 C═NOH formation in an aqueous medium. Upon incorporating into a flow electrolyzer, the yield rate for H 2 C═NOH electrosynthesis is drastically enhanced to 2630 mmol h −1  g −1 , almost triple that obtained from H‐cell setups. Our techno‐economic analysis estimates that the daily profit of this dual‐upgrading technology reaches $230 000+, highlighting the translational advantage of our strategy. Overall, this work establishes a non‐precious metal‐dopant strategy that upcycles low‐cost C‐ and N‐containing pollutants into valuable organonitrogens, enabling renewable energy synthesis of more valuable and functionally diverse commodities.