High-entropy perovskites, architectured by s0/d0/d10 cations, as novel electrolytes for solid oxide fuel cells

Original · EN

Solid oxide fuel cells enable efficient conversion of hydrogen into electricity. However, the limited availability of materials for their cathode, anode, and electrolyte remains a concern. This study introduces three high-entropy oxide perovskites as novel electrolyte materials for fuel cells (Ba0.50Sr0.50)(Ti0.33Zr0.33Hf0.33)O3 with s0/d0 cations, (Ba0.50Sr0.50)(Ga0.33In0.33Sn0.33)O3 with s0/d10 cations, and (Ba0.50Sr0.50)(Ti0.33Zr0.33Sn0.33)O3 with mixed s0/d0/d10 cations. Through sequential sintering by high-pressure torsion processing and calcination, these perovskites were synthesized and then printed with a thickness of about 6-10 microns on a Ni-SrZr0.5Ce0.4Y0.1O3 substrate as an anode and then coated with Ba0.5La0.5CoO3 as a cathode. Electrochemical analysis and impedance spectroscopy show that (Ba0.50Sr0.50)(Ti0.33Zr0.33Sn0.33)O3 with s0/d0/d10 cations exhibits the best performance with negligible current leakage and lowest ohmic resistance, while its maximum power density reaches 0.53 W.cm-2 at 973 K. Complementary synchrotron X-ray absorption and photoelectron spectroscopy analyses indicate that the superior performance of (Ba0.50Sr0.50)(Ti0.33Zr0.33Sn0.33)O3 correlates with its heterogeneous electronic structure characterized by tailored unoccupied d-orbital states, and favorable local metal-oxygen bond lengths and extrinsic oxygen vacancies. This investigation demonstrates the significance of high-entropy perovskites with mixed s0/d0/d10 cations as new rare-earth metal-free ion-conducting electrolytes, particularly for protonic solid oxide fuel cells.