Redefining electrochemical C–N coupling via electrolyte engineering

Electrochemical synthesis offers a promising route powered by renewable electricity toward sustainable chemical manufacturing.Among the various electrosynthetic transformations reported thus far, C-N bond formation is particularly attractive because it enables the production of value-added chemicals like urea, amides, amines, and amino acids under mild conditions [1][2][3][4] .Compared with conventional thermochemical synthetic techniques, electrochemical C-N coupling offers several advantages, including operation under ambient conditions, modular reactor design, and compatibility with distributed energy systems.However, achieving selective and efficient C-N bond formation by electrosynthesis remains challenging because the reaction involves multiple competing pathways and highly reactive intermediates that are difficult to coordinate at the catalytic interface.To date, electrochemical C-N coupling has been studied largely using a catalystcentered framework, with major research efforts devoted to defect engineering, facet modulation, heterostructure construction, and active-site regulation [5][6][7] .Although these strategies have substantially improved catalytic performance, the catalyst surface J u s t A c c e p t e d Future Carbon Future (1-x)Carbon Future, 2026, 3, 9200086 represents only one component of the dynamic electrochemical interface.Catalyst surfaces fundamentally determine adsorption configurations, electronic structures, and accessible reaction pathways, while the surrounding electrolyte regulates the local environment in which these surface reactions occur.Electrochemical C-N coupling should therefore be understood as an interface-driven process governed by the cooperative effects of the catalyst and electrolyte.At such interfaces, reactant transport, solvation organization, proton availability, interfacial electric fields, and intermediate