Highly Stable Garnet Fe₂Mo₃O₁₂ Cathode Boosts the Lithium–Air Battery Performance Featuring a Polyhedral Framework and Cationic Vacancy Concentrated Surface

Abstract

Lithium-air batteries (LABs), owing to their ultrahigh theoretical energy density, are recognized as one of the next-generation energy storage techniques. However, it remains a tricky problem to find highly active cathode catalyst operating within ambient air. In this contribution, a highly active Fe₂ Mo₃ O₁₂ (FeMoO) garnet cathode catalyst for LABs is reported. The experimental and theoretical analysis demonstrate that the highly stable polyhedral framework, composed of FeO octahedrons and MO tetrahedrons, provides a highly effective air catalytic activity and long-term stability, and meanwhile keeps good structural stability. The FeMoO electrode delivers a cycle life of over 1800 h by applying a simple half-sealed condition in ambient air. It is found that surface-rich Fe vacancy can act as an O₂ pump to accelerate the catalytic reaction. Furthermore, the FeMoO catalyst exhibits a superior catalytic capability for the decomposition of Li₂ CO₃ . H₂ O in the air can be regarded as the main contribution to the anode corrosion and the deterioration of LAB cells could be attributed to the formation of LiOH·H₂ O at the end of cycling. The present work provides in-depth insights to understand the catalytic mechanism in air and constitutes a conceptual breakthrough in catalyst design for efficient cell structure in practical LABs.