Abstract
The practical application of Li-S battery is severely hampered by the sluggish sulfur-related redox reaction (SROR) kinetics along with lithium polysulfides (LiPSs) shuttle effect, advanced single-atom catalyst (SAC) is pursued to improve the SROR conversion capability. Herein, a novel SAC possessing of high loading (3.02 wt%) atomically dispersed Fe five-coordinated with pyridinic and pyrrolic N anchored on porous N-rich (16.4 at.%) carbon matrix is obtained. The resultant Fe-N5/NC SAC has a high Brunauer-Emmett-Teller surface area of 523 m2 g−1. The unique asymmetrical Fe-N5 sites in Fe-N5/NC are identified by spherical aberration-corrected high-angle annular dark-field scanning transmission electron microscope, X-ray photoelectron spectroscope, synchrotron X-ray absorption spectroscopy, density functional theory calculation, etc. The experimental and theoretical results demonstrate that the Fe-N5/NC SAC not only exhibits strong adsorption for LiPSs, but also provides a significant electrocatalytic effect on the SROR in Li-S battery. A high initial capacity of 1519 mAh g−1 was obtained at a current density of 0.1 C for the Li-S battery based on the Fe-N5/NC modified separator. An ultralong life of 2000 cycles was achieved for the Li-S battery, which has good initial capacities of 1030 mAh g−1 and 883 mAh g−1 with low decay rates of 0.032% and 0.031% per cycles at 1 C and 2 C, respectively.
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