Functional Zoning Cobalt Synergistically Promotes Ammonia Synthesis

Abstract Electrocatalytic reduction of nitrate to ammonia is an important means for the future from nitrogen to ammonia products, but the multi‐reaction coexistence and complex reaction process depend on the input of highly active catalysts. By introducing a long alkyl chain as a morphology inducer, one‐step electrodeposition promoted the cross‐arrangement of multi‐type cobalt species nanosheets on the surface of carbon fibers, and developed a self‐supporting high‐activity eNitRR catalyst (CoO/Co/CF) that can be applied to large‐scale rapid manufacturing in industry. CoO/Co/CF demonstrates efficient NO 3 − to NH 3 conversion various working conditions, achieving a Faradaic efficiency close to 100%, while maintaining robust electrocatalytic stability. A high‐performance Zn‐nitrate battery was built based on CoO/Co/CF, and an energy storage and conversion system for self‐driven ammonia synthesis and energy supply was established; The cascade process from air to nitrogen oxides to ammonia is established, and the demonstration from solar energy to ammonia products is realized, which fully adapts to the pattern of distributed industrial and agricultural production in the future. Furthermore, this study provides comprehensive experimental and theoretical evidence that the establishment of functionally partitioned cobalt species effectively addresses the challenges of multi‐reaction coexistence and complex hydrogenation pathways in eNitRR, and establishes a paradigm for cascade/synergistic catalysis.