Gram‐Scale Ammonia Synthesis via Electrochemical Nitrate Reduction Using Enzyme‐Inspired Dual‐Atomic Cu Catalyst

Abstract The potential application prospects of green electricity‐driven electrocatalytic nitrate reduction (NO₃RR) technology for the production of valuable ammonia have garnered widespread attention. However, designing electrocatalysts with remarkable activity and stability for the NO₃RR to realize gram‐level ammonia production remains a significant hurdle in terms of practical application. In nature, the synergistic effect of the dual‐site copper of nitrite reductase promotes the substrate adsorption and protonation, achieving efficient conversion of nitrite. Herein, enzyme‐inspired Cu dual‐atomic sites are constructed on polymeric carbon nitride (PCN‐Cu‐DAC). Systematic investigations indicate the dual‐atomic Cu sites in the catalyst exhibit stronger proton transfer and synergistic nitrate adsorption interaction, thereby reducing the energy barrier for *NO protonation. Studies have shown that the PCN‐Cu‐DAC catalyst presents a remarkable ammonia (NH₃) yield (467 mg h −1 mg −1 cat. and 102 mg h −1 cm −2 ) and achieves 11 g d −1 NH₃ yield at 6 A of current for 360 h. This work demonstrates the concept of mimicking natural nitrite reductase toward the continuous reduction of nitrate wastewater and promotes the production of NH 3 .