The electrochemical N 2 reduction reaction has attracted interest as a potential alternative to the Haber−Bosch process, but a significantly low conversion efficiency and a significantly low ammonia production rate stimulate the need for alternatives. Here, we represent the electrochemical reduction of nitric oxide (NO) on a nanostructured Ag electrode in combination with a rationally designed electrolyte containing the EDTA−Fe 2+ metal complex (EFeMC), which results in an ∼100% efficiency for NH 3 with a current density of 50 mA/cm 2 at −0.165 V RHE , without any degradation in catalytic activity or product selectivity up to 120 h. Economic analysis using itemized cost estimation predicted that the synthesis of ammonia from NO reduction in an EFeMC-designed electrolyte can be market competitive at an electricity price of $0.03 kWh −1 with a current density of >125 mA/cm 2 . Therefore, this approach opens an entirely new avenue of renewable electricitydriven ammonia synthesis.

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