NO3− is a prominent waste byproduct in ammunition industries, and valorization of NO3− into NH3 is desired. NH3 synthesized from waste using renewable energy could be used as an energy storage medium. For such a process, higher selectivity, stability, and enhanced activity per unit mass of catalyst is required. This work reports CoO nanoclusters functionalized on graphene as an efficient catalyst for electrochemical NO3− reduction to NH3 with >98% NH3 Faradaic efficiency and an NH3 current density (geometric) of ≈400 mA cm−2. A highest NH3 yield of 25.63 mol g−1 h−1 is obtained. The developed catalyst prevents the NN coupling step which is required for promoting the selectivity of NH3 over N2. Density functional theory calculations reveal that CoO NC/graphene has similar selectivity to that of polycrystalline Co and that higher activity can be obtained with lower catalyst loading.

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