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Reversible solid oxide cells (RSOCs) present a conceivable potential for addressing energy storage and conversion issues through realizing efficient cycles between fuels and electricity based on the reversible operation of the fuel cell (FC) mode and electrolysis cell (EC) mode. Reliable electrode materials with high electrochemical catalytic activity and sufficient durability are imperatively desired to stretch the talents of RSOCs. Herein, oxygen vacancy engineering is successfully implemented on the Fe-based layered perovskite by introducing Zr4+, which is demonstrated to greatly improve the pristine intrinsic performance, and a novel efficient and durable oxygen electrode material is synthesized. The substitution of Zr at the Fe site of PrBaFe2O5+δ (PBF) enables enlarging the lattice free volume and generating more oxygen vacancies. Simultaneously, the target material delivers more rapid oxygen surface exchange coefficients and bulk diffusion coefficients. The performance of both the FC mode and EC mode is greatly enhanced, exhibiting an FC peak power density (PPD) of 1.26 W cm–2 and an electrolysis current density of 2.21 A cm–2 of single button cells at 700 °C, respectively. The reversible operation is carried out for 70 h under representative conditions, that is, in air and 50% H2O + 50% H2 fuel. Eventually, the optimized material (PBFZr), mixed with Gd0.1Ce0.9O2, is applied as the composite oxygen electrode for the reversible tubular cell and presents excellent performance, achieving 4W and 5.8 A at 750 °C and the corresponding PPDs of 140 and 200 mW cm–2 at 700 and 750 °C, respectively. The enhanced performance verifies that PBFZr is a promising oxygen electrode material for the tubular RSOCs.

Intermediate temperature solid oxide fuel cells (IT-SOFCs) have been extensively studied due to high efficiency, cleanliness, and fuel flexibility. To develop highly active and stable IT-SOFCs for the practical application, preparing an efficient cathode is necessary to address the challenges such as poor catalytic activity and CO2 poisoning. Herein, an efficient optimized strategy for designing a high-performance cathode is demonstrated. By motivating the phase transformation of BaFeO3‑δ perovskites, achieved by doping Pr at the B site, remarkably enhanced electrochemical activity and CO2 resistance are thus achieved. The appropriate content of Pr substitution at Fe sites increases the oxygen vacancy concentration of the material, promotes the reaction on the oxygen electrode, and shows excellent electrochemical performance and efficient catalytic activity. The improved reaction kinetics of the BaFe0.95Pr0.05O3‑δ (BFP05) cathode is also reflected by a lower electrochemical impedance value (0.061 Ω·cm2 at 750 °C) and activation energy, which is attributed to high surface oxygen exchange and chemical bulk diffusion. The single cells with the BFP05 cathode achieve a peak power density of 798.7 mW·cm–2 at 750 °C and a stability over 50 h with no observed performance degradation in CO2-containing gas. In conclusion, these results represent a promising optimized strategy in developing electrode materials of IT-SOFCs.

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Solid oxide electrolysis cells (SOECs) have emerged as one of the most potent techniques for hydrogen production. As the restricted step for SOEC, as well as the most predominant obstacle to the scaled application, oxygen evolution reaction (OER) should be urgently accelerated by developing potent electrocatalysts. Despite inferior electrochemical activity to cobalt-based materials, perovskite ferrites exhibit great potential in the future with regard to good intrinsic stability and durability, abundant reserves, and good compatibility with other SOEC components. In this work, fluorination is introduced to the typical perovskite ferrite to further intensify the OER process. Ab initio calculations combined with physical–chemical characterizations are performed to reveal the mechanism. The doped F − leads to debilitating the strength of the metal–oxygen bond and then reduces the energy for oxygen vacancy formation and ion migration, which renders improvements to sub-processes of OER on the anode. The well-verified material, PrBaFe 2 O 5+δ F 0.1 (PBFOF), exhibited a low polarization resistance of 0.058 Ω cm −2 . Single cells based on PBFOF showed a high current density of 2.28 A cm −2 at 750 °C under 1.3 V. This work provides a clear insight into the mechanism of fluorination on perovskites and high-activity anode material for SOEC.