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.