Efficient Polysulfide Redox Enabled by Lattice-Distorted Ni₃Fe Intermetallic Electrocatalyst-Modified Separator for Lithium–Sulfur Batteries

Exploring efficient electrocatalysts for lithium–sulfur (Li–S) batteries is of great significance for the sulfur/polysulfide/sulfide multiphase conversion. Herein, we report nickel–iron intermetallic (Ni3Fe) as a novel electrocatalyst to trigger the highly efficient polysulfide-involving surface reactions. The incorporation of iron into the cubic nickel phase can induce strong electronic interaction and lattice distortion, thereby activating the inferior Ni phase to catalytically active Ni3Fe phase. Kinetics investigations reveal that the Ni3Fe phase promotes the redox kinetics of the multiphase conversion of Li–S electrochemistry. As a result, the Li–S cells assembled with a 70 wt % sulfur cathode and a Ni3Fe-modified separator deliver initial capacities of 1310.3 mA h g–1 at 0.1 C and 598 mA h g–1 at 4 C with excellent rate capability and a long cycle life of 1000 cycles at 1 C with a low capacity fading rate of ∼0.034 per cycle. More impressively, the Ni3Fe-catalyzed cells exhibit outstanding performance even at harsh working conditions, such as high sulfur loading (7.7 mg cm–2) or lean electrolyte/sulfur ratio (∼6 μL mg–1). This work provides a new concept on exploring advanced intermetallic catalysts for high-rate and long-life Li–S batteries.