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Reactive nitrogen (Nr) is an essential nutrient to life on earth, but its mismanagement in waste has emerged as a major problem in water pollution to our ecosystems, causing severe eutrophication and health concerns. Sustainably recovering Nr [such as nitrate (NO3−)–N] and converting it into ammonia (NH3) could mitigate the environmental impacts of Nr, while reducing the NH3 demand from the carbon-intensive Haber–Bosch process. In this work, high-performance NO3−-to-NH3 conversion was achieved in a scalable, versatile, and cost-effective membrane-free alkaline electrolyzer (MFAEL): a remarkable NH3partial current density of 4.22 ± 0.25 A cm−2 with a faradaic efficiency of 84.5 ± 4.9%. The unique configuration of MFAEL allows for the continuous production of pure NH3-based chemicals (NH3 solution and solid NH4HCO3) without the need for additional separation procedures. A comprehensive techno-economic analysis (TEA) revealed the economic competitiveness of upcycling waste N from dilute sources by combining NO3− reduction in MFAEL and a low-energy cost electrodialysis process for efficient NO3− concentration. In addition, pairing NO3− reduction with the oxidation of organic Nr compounds in MFAEL enables the convergent transformation of N–O and C–N bonds into NH3 as the sole N-containing product. Such an electricity-driven process offers an economically viable solution to the growing trend of regional and seasonal Nr buildup and increasing demand for sustainable NH3 with a reduced carbon footprint.more » « less
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