The electroreduction of nitrate to ammonia is both an alternative strategy to industrial Haber-Bosch ammonia synthesis and a prospective idea for changing waste (nitrate pollution of groundwater around the world) into valuable chemicals, but still hindered by its in-process strongly competitive hydrogen evolution reaction (HER), low ammonia conversion efficiency, and the absence of stability and sustainability. Considering the unique electronic structure of anti-perovskite structured FeN, a tandem disproportionation reaction and nitridation-carbonation route for building a multi-layer core-shell oxide/nitride/C catalyst, such as MoO/FeN/C, is designed and executed, in which abundant Fe-N active sites and rich phase interfaces are formed for both suppressing HER and fast transport of electrons and reaction intermediates. As a result, the sample's NORR conversion displays a very high NH yield rate of up to 11.10 mol g h (1.67 mmol cm h) with a superior 99.3% faradaic efficiency and the highest half-cell energy efficiency of 30%, surpassing that of most previous reports. In addition, it is proved that the NORR assisted by the MoO/FeN/C electrocatalyst can be carried out in 0.50-1.00 M KNO electrolyte at a pH value of 6-14 for a long time. These results guide the rational design of highly active, selective, and durable electrocatalysts based on anti-perovskite FeN for the NORR.
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