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

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 MoS₂ as efficient catalysts. Notably, Fe-doped MoS₂ significantly boosts the Faradaic efficiency and yield rate for H₂C═NOH to 81.2% and 963 mmol h^-1 g^-1, respectively. Mechanistic studies reveal that the Fe dopants enhance the NO₂ ^- bonding, promoting substrate engagement and subsequently H₂C═NOH formation in an aqueous medium. Upon incorporating into a flow electrolyzer, the yield rate for H₂C═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.