Bioinspired Fe/Mn Dual‐Atom Catalysts with Mesoporous Channels for Rapid Polysulfide Redox Kinetics and Stable Lithium–Sulfur Batteries

Superoxide dismutase-inspired carbon cathode with mesoporous channels and Fe/Mn dual-atom sites has been proposed for accelerating sulfur redox kinetics. The Fe sites act as redox-active centers, directly mediating electron transfer through a reversible Fe²⁺/Fe³⁺ cycle to drive efficient polysulfide interconversion. Complementally, Mn regulates the catalytic process via stabilizing the architecture and transferring Li⁺, which resulted in enhanced battery performance.

The sluggish sulfur redox kinetics and severe polysulfide shuttling significantly hinder the practical performance of lithium–sulfur batteries (LSBs). While single-atom catalysts have shown promise in capturing and catalyzing sulfur species, their catalytic activity still requires further enhancement for real-world applications. Inspired by natural superoxide dismutase, which utilizes dual-atom catalytic sites and a synergistic mechanism for rapid substrate conversion, a bioinspired Fe/Mn dual-atom catalyst (FeMn-DAC) anchored on nanochannel-decorated carbon to improve sulfur redox kinetics and enable high-performance LSBs is developed. Experimental results reveal that LSBs equipped with FeMn-DACs electrocatalyst exhibit the fastest nucleation (369.3 mAh g⁻¹) and dissolution (226.3 mAh g⁻¹) kinetics of Li₂S. The battery demonstrates outstanding rate performance, delivering a reversible capacity of 670 mAh g⁻¹ at 2.0C, coupled with an ultralow capacity decay rate of 0.09% over 500 cycles. Even under high-sulfur loadings of 2.79and 3.67 mg cm⁻², the FeMn-DACs-based cathodes achieve excellent area capacities of 2.06 and 2.69 mAh cm⁻², respectively. This work provides a new perspective for designing advanced DACs tailored for LSBs.

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