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 e g filling and induce a high-to-medium spin transition of Fe 3+ 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.
Carbon-doped SiO2 is synthesized by the in situ carbonization of halloysite. Carbon atoms partially substitute O atoms to form Si-C bonds and manipulate the localized electronic states of Si atoms,...
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