Publication date: 15th December 2025
Ammonia has attracted increasing attention as a carbon-free energy carrier owing to its high hydrogen density and favorable liquefaction characteristics compared to molecular hydrogen. Despite its industrial maturity, the Haber–Bosch process remains intrinsically energy-intensive due to its reliance on high temperature and pressure operation, motivating the development of alternative ammonia synthesis pathways under ambient conditions. Among them, Li-mediated electrochemical nitrogen reduction has emerged as a promising route, yet its practical implementation is fundamentally constrained by the incompatibility between lithium-mediated N₂ activation and aqueous proton sources.
Here, we demonstrate a reaction architecture that decouples lithium-mediated nitrogen activation from proton delivery, enabling the use of water-derived protons without destabilizing the Li–N₂ chemistry. This is achieved through a biphasic electrolyte configuration comprising an organic-phase catholyte and an aqueous-phase anolyte, separated by a cross-linked anion exchange membrane that selectively facilitates proton transport while suppressing water permeation. The resulting system sustains stable ammonia generation for 50 h with a Faradaic efficiency of approximately 60%.
By mitigating the long-standing incompatibility between lithium reactivity and water-based proton sources, this work demonstrates the feasibility of integrating aqueous chemistry into Li-mediated nitrogen reduction systems, while highlighting remaining challenges in long-term stability.
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