Enhanced Electrochemical Performance of the Fe-Based Layered Perovskite Oxygen Electrode for Reversible Solid Oxide...

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 PrBaFe₂O_5+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 Gd_0.1Ce_0.9O₂, 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.