Smart Compositional Design of B-Site Ordered Double Perovskite for Advanced Oxygen Catalysis at Ultra-High Current Densities

Perovskite oxides have been considered promising oxygen catalysts for oxygen reduction and evolution reactions (ORR and OER), owing to structural and compositional flexibility, and tailorable properties. Ingenious B-site ordered La Sr NiMn Fe O (LSNMF) double perovskite is strategically designed by simultaneously interposing Ni Mn and Ni Fe into B' and B″ sites. Controlling B-site cation systematically tailors the electronic structure of the B-site cation with a d-band center (M ) upshift close to the Fermi level, increasing the overlap of the M center and O 2p center (O ). The strong interaction of M and O facilitates the adsorption of oxygen and activates the lattice oxygen to participate in the OER process, thereby enhancing the ORR and OER activity. For ORR, LSNMF exhibited an onset potential of 0.9 V along with a high limiting current of -8.05 mA cm . At the same time, for OER at 1 m KOH, LSNMF effectively reached a maximum current density of 3000 mA cm . Most importantly, the difference between E (at -1 mA cm ) and E (at 10 mA cm ), ΔE is 0.69 V, which stands among the best of recently reported perovskites. The as-designed LSNMF is stable, efficient, lucrative, and a promising candidate for practical application.