Highly Stable Perovskite Oxides for Electrocatalytic Acidic NOx - Reduction Streamlining Ammonia Synthesis from Air.

ABSTRACT

Electrochemical nitrogen oxide ions reduction reaction (NOx -RR) shows great opportunity for ammonia production under ambient conditions. Yet, performing NOx -RR in strong acidic conditions remains challenging due to the corrosion effect on the catalyst and competing hydrogen evolution reactions. Here, we demonstrate a stable La1.5Sr0.5Ni0.5Fe0.5O4 perovskite oxide for the NOx -RR at pH 0, achieving a Faradaic efficiency for ammonia of approaching 100 % at a current density of 2 A cm-2 in a H-type cell. At industrially relevant current density, the NOx -RR system shows stable cell voltage and Faradaic efficiency for >350 h in membrane electrode assembly (MEA) at pH 0. By integrating the catalyst in a stacked MEA with a series connection, we have successfully obtained a record-breaking 2.578 g h-1 NH3 production rate at 20 A. This catalyst's unique acid-operability streamlines downstream ammonia utilization for direct ammonium salt production and upstream integration with NOx sources. Techno-economic and lifecycle assessments reveal substantial economic advantages for this ammonia production strategy, even when coupled with a plasma-based NOx production system, presenting a sustainable complement to the conventional Haber-Bosch process.