Perovskite Oxynitrides for Plasma-Driven Ammonia Synthesis: Unlocking the Potential of Lattice Nitrogen under Mild Conditions

Abstract

Plasma ammonia synthesis driven by renewable electrical energy has the advantage of being cleaner and more distributed than the traditional Haber-Bosch process, which offers greater flexibility in material selection and process innovation for nitrogen fixation due to the unique catalytic environment. Inspired by the classical Mars and Van Krevelen (MvK) mechanism, we present a plasma-assisted lattice nitrogen ammonia synthesis strategy based on oxynitride perovskites, which improves the efficiency of utilizing plasma-excited species. It enables separated plasma hydrogenation and lattice nitrogen replenishment processes, achieving the highest rate (7087 μmol/gcat/h) of plasma ammonia synthesis to date. This strategy greatly extends the application range of the plasma tandem ammonia synthesis process and provides new ideas for the design of plasma-catalyzed conversion systems.