Ni-Doped SFM Double-Perovskite Electrocatalyst for High-Performance Symmetrical Direct-Ammonia-Fed Solid Oxide Fuel Cells

Ammonia has emerged as a promising fuel for solid oxide fuel cells (SOFCs) owing to its high energy density, high hydrogen content, and carbon-free nature. Herein, the electrocatalytic potential of a novel Ni-doped SFM double-perovskite (Sr_1.9Fe_0.4Ni_0.1Mo_0.5O_6-δ) is studied, for the first time, as an alternative anode material for symmetrical direct-ammonia SOFCs. Scanning and transmission electron microscopy characterization has revealed the exsolution of Ni-Fe nanoparticles (NPs) from the parent Sr₂Fe_1.5Mo_0.5O₆ under anode conditions, and X-ray diffraction has identified the FeNi₃ phase after exposure to ammonia at 800 °C. The active-exsolved NPs contribute to achieving a maximal ammonia conversion rate of 97.9% within the cell's operating temperatures (550-800 °C). Utilizing 3D-printed symmetrical cells with SFNM-GDC electrodes, the study demonstrates comparable polarization resistances and peak power densities of 430 and 416 mW cm^-2 for H₂ and NH₃ fuels, respectively, with long-term stability and a negligible voltage loss of 0.48% per 100 h during ammonia-fed extended galvanostatic operation. Finally, the ammonia consumption mechanism is elucidated as a multistep process involving ammonia decomposition, followed by hydrogen oxidation. This study provides a promising avenue for improving the performance and stability of ammonia-based SOFCs for potential applications in clean energy conversion technologies.