Rational Design of Ruddlesden–Popper Perovskite Ferrites as Air Electrode for Highly Active and Durable Reversible Protonic Ceramic Cells

Reversible protonic ceramic cells (RePCCs) hold promise for efficient energy storage, but their practicality is hindered by a lack of high-performance air electrode materials. Ruddlesden–Popper perovskite Sr₃Fe₂O_7−δ (SF) exhibits superior proton uptake and rapid ionic conduction, boosting activity. However, excessive proton uptake during RePCC operation degrades SF’s crystal structure, impacting durability. This study introduces a novel A/B-sites co-substitution strategy for modifying air electrodes, incorporating Sr-deficiency and Nb-substitution to create Sr_2.8Fe_1.8Nb_0.2O_7−δ (D-SFN). Nb stabilizes SF's crystal, curbing excessive phase formation, and Sr-deficiency boosts oxygen vacancy concentration, optimizing oxygen transport. The D-SFN electrode demonstrates outstanding activity and durability, achieving a peak power density of 596 mW cm⁻² in fuel cell mode and a current density of − 1.19 A cm⁻² in electrolysis mode at 1.3 V, 650 °C, with excellent cycling durability. This approach holds the potential for advancing robust and efficient air electrodes in RePCCs for renewable energy storage. (Figure presented.)