Nitrogen Coordinated Fe‐Co Diatomic Catalyst Enabling High Energy Density Li‐S Pouch Cells via Bifunctional Electrocatalysis

ABSTRACT Rational design of efficient electrocatalysts to regulate sulfur redox kinetics is crucial for inhibiting “shuttle effect” in practical Li‐S batteries under high sulfur loading and lean electrolyte conditions. Herein, we synthesize a nitrogen‐coordinated porous carbon supported FeCo diatomic catalyst as a bifunctional sulfur host. Fe and Co centers exhibit asymmetric electron distribution and synergistic interactions, enabling selective acceleration of sulfur reduction at Fe sites and Li 2 S oxidation at Co sites. Combined experimental and theoretical analyses collectively validate this bifunctional catalytic mechanism, which significantly improves sulfur redox reversibility and inhibits polysulfide shuttling. Consequently, the FeCo DA‐NC based Li‐S coin cells deliver ultra‐high sulfur utilization (1616 mAh g −1 at 0.1 C), superior rate capability (912 mAh g −1 at 2 C) and stable cycling (714 mAh g −1 after 500 cycles at 1.0 C). Even under harsh conditions (7.8 mg cm −2 , E/S = 5.0 µL mg s −1 ), 83.3% capacity retention is maintained after 100 cycles at 0.1 C. And the FeCo DA‐NC based 8 Ah‐level Li‐S pouch cell achieves a high energy density of 480 Wh kg −1 . Overall, this work provides the first demonstration of diatomic catalyst strategy in practical Li‐S pouch cells, establishing a viable pathway for future Li‐S batteries.