Cascade electrosynthesis of LiTFSI and N-containing analogues via a looped Li–N₂ battery

The synthesis of N-containing chemicals directly from N₂ is highly desirable in chemistry but has been challenged by inert N₂ molecules and limited product scope. Herein we propose a cascade electrosynthesis strategy for the facile reduction of N₂ and subsequent conversion to various N-containing chemicals via a looped Li–N₂ battery. The electrosynthesis of lithium bis(trifluoromethanesulfonyl)imide is illustrated as a prototype using cascade reactions involving electrocatalytic N₂ reduction to Li₃N on discharge, a relay reaction of Li₃N acylation to lithium bis(trifluoromethanesulfonyl)imide and finally the elimination of the LiCl by-product on charge to complete the synthesis loop. This strategy provides direct access to analogues with different N–X bonds (X = S, C and so on) and metal cations (Li⁺, Zn²⁺ and so on) by extending the substrate scope, and can be scaled up for improved energy efficiency and atom economy. This work provides a general electrosynthesis protocol for the practical production of N-containing chemicals and has potential implications for a wider field of sustainable chemistry.