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Abstract A glut of dinitrogen‐derived ammonia (NH₃) over the past century has resulted in a heavily imbalanced nitrogen cycle and consequently, the large‐scale accumulation of reactive nitrogen such as nitrates in our ecosystems has led to detrimental environmental issues. Electrocatalytic upcycling of waste nitrogen back into NH₃holds promise in mitigating these environmental impacts and reducing reliance on the energy‐intensive Haber–Bosch process. Herein, we report a high‐performance electrolyzer using an ultrahigh alkalinity electrolyte, NaOH−KOH−H₂O, for low‐cost NH₃electrosynthesis. At 3,000 mA/cm², the device with a Fe−Cu−Ni ternary catalyst achieves an unprecedented faradaic efficiency (FE) of 92.5±1.5 % under a low cell voltage of 3.83 V; whereas at 1,000 mA/cm², an FE of 96.5±4.8 % under a cell voltage of only 2.40 V was achieved. Techno‐economic analysis revealed that our device cuts the levelized cost of ammonia electrosynthesis by ~40 % ($30.68 for Fe−Cu−Ni vs. $48.53 for Ni foam per kmol‐NH₃). The NaOH−KOH−H₂O electrolyte together with the Fe−Cu−Ni ternary catalyst can enable the high‐throughput nitrate‐to‐ammonia applications for affordable and scalable real‐world wastewater treatments. 

Greenhouse gas emissions present a significant challenge to humanity, and utilizing renewable electricity to convert emitted CO2 into value-added products offers a promising solution; however, traditional CO2 capture and regeneration processes remain energy-intensive, restricting the overall system efficiency and decarbonization efficacy. In this study, an advanced direct reduction of captured CO2 with large current densities for formate electrosynthesis was demonstrated without the need for CO2 regeneration or compression. The bismuth nanosheet (DRM-BiNS) was synthesized by direct reduction of a Bi-based MOF, representing a new class of catalytic materials with a large surface area and interconnected pores, suitable for the direct reduction of captured CO₂. By seamlessly combining experimentation and simulation, insights into the structure-parameter-performance relation were acquired in a flow cell setting, including critical membrane-electrode distance, cell orientation, and pumping flow rate. Important flow-cell components, such as catholyte volume, electrode substrate, membrane choice, and ionomer type, were also carefully examined to enhance the cell performance. In sharp contrast to prior studies limited to current densities below 20 mA/cm² in bicarbonate-based captured CO2 solutions, this work demonstrates a remarkable current density of 300 mA/cm² with an FE to formate comparable to the case with gas-fed CO2 reduction. Moreover, the process sustained an FE above 50% at a high current density of 500 mA/cm². The DRM-BiNS catalyst exhibited outstanding selectivity, activity, and stability, significantly outperforming oxide-derived bismuth nanosheets (OD-BiNS) in captured CO2 reduction. These findings offer critical insights into the development of sustainable and scalable CO2 utilization technologies. 

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.