Abstract
The issues of polysulfide shuttling and lethargic sulfur redox reaction (SROR) kinetics are the toughest obstacles of lithium-sulfur (Li-S) battery. Herein, integrating the merits of increased density of metal sites and synergistic catalytic effect, a unique single-atom catalyst (SAC) with nonmetallic-bonding Fe-Mn diatomic pairs anchored on hollow nitrogen-doped carbonaceous nanodisk (denoted as FeMnDA@NC) is successfully constructed and well characterized by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, X-ray absorption spectroscopy, etc. Density functional theory calculation indicates that the Fe-Mn diatomic pairs can effectively inhibit the shuttle effect by enhancing the adsorption ability retarding the polysulfide migration and accelerate the SROR kinetics. As a result, the Li-S battery assembled with FeMnDA@NC modified separator possesses an excellent electrochemical performance with ultrahigh specific capacities of 1419 mAh g-1 at 0.1 C and 885 mAh g-1 at 3.0 C, respectively. An outstanding specific capacity of 1165 mAh g-1 is achieved at 1.0 C and maintains at 731 mAh g-1 after 700 cycles. Notably, the assembled Li-S battery with a high sulfur loading of 5.35mg cm-2 harvests a practical areal capacity of 5.70 mAh cm-2 at 0.2 C. A new perspective is offered here to construct advanced SACs suitable for the Li-S battery.
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