Highly efficient electrochemical ammonia synthesis via nitrate reduction over metallic Cu phase coupling sulfion oxidation

Electrochemical nitrate reduction reaction (NO3RR) is a promising technology for ammonia production and denitrification of wastewater. Its application is seriously restricted by the development of the highly active and selective electrocatalyst and a rational electrolysis system. Here, we constructed an efficient electrochemical ammonia production process via nitrate reduction on the metallic Cu electrocatalyst when coupled with anodic sulfion oxidation reaction (SOR). The synthesized Cu catalyst delivers an excellent NH3 Faradaic efficiency of 96.0 % and a NH3 yield of 0.391 mmol h-1 cm-2 at -0.2 V vs. reversible hydrogen electrode, which mainly stem from the more favorable conversion of NO2- to NH3 on Cu0. Importantly, the well-designed electrolysis system with cathodic NO3RR and anodic SOR achieves a dramatically reduced cell voltage of 0.8 V at 50 mA cm-2 in comparison with the one with anodic oxygen evolution reaction (OER) of 1.9 V. This work presents an effective strategy for the energy-saving ammonia production via constructing effective nitrate reduction catalyst and replacing the OER with SOR while removing the pollutants including nitrate and sulfion. The efficient nitrate reduction to ammonia on metallic Cu phase was realized. The cell voltage was significantly reduced through an energy-saving ammonia production system of cathodic nitrate reduction reaction (NO3RR) and anodic sulfion oxidation reaction (SOR) rather than oxygen evolution reaction (OER). Note that the efficient ammonia synthesis can be driven by a 1.2 V commercial battery.+ image