Manipulating the Spin State of Fe Sites via Fe–O–Si Bridge Bonds for Enhanced Polysulfide Redox Kinetics in the Li–S Battery

Transition metals with 3d unoccupied orbitals have superior catalytic activity, but inherent high spin suppresses their adsorption capability, leading to sluggish polysulfide conversion kinetics for Li-S batteries. Herein, we provide Fe-O-Si bridge bonds to manipulate eg filling and induce a high-to-medium spin transition of Fe3+ sites, which enhances polysulfide adsorption and facilitates sulfur redox reaction kinetics. The resultant cathodes exhibit outstanding performances under high sulfur loading, which can deliver a high battery specific energy of 1061 mA h·g-1 even after 100 cycles in Li-S pouch batteries. This work provides new insights into the kinetic and multi-step conversion mechanism of the sulfur redox reaction process, helping in the understanding and design of spin-dependent catalysts.