Journal
ACS NANO
Volume 14, Issue 8, Pages 10115-10126Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c03325
Keywords
Li-S battery; lithium polysulfide conversion; atomically dispersed catalyst; energy storage; electrocatalysis
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Funding
- National Materials Genome Project [2016YFB0700600]
- National Nature Science Foundation of China [21972051]
- Graduates' Innovation Fund, Huazhong University of Science and Technology [2019ygscxcy031]
- U.S. National Science Foundation [DMR1828019]
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The sluggish kinetics of lithium polysulfides (UPS) transformation is recognized as the main obstacle against the practical applications of the lithium-sulfur (Li-S) battery. Inspired by molybdoenzymes in biological catalysis with stable Mo-S bonds, porous Mo-N-C nanosheets with atomically dispersed Mo-N-2/C sites are developed as a S cathode to boost the LiPS adsorption and conversion for Li-S batteries. Thanks to its high intrinsic activity and the Mo-N-2/C coordination structure, the rate capability and cycling stability of S/Mo-N-C are greatly improved compared with S/N-C due to the accelerated kinetics and suppressed shuttle effect. The S/Mo-N-C delivers a high reversible capacity of 743.9 mAh g(-1) at 5 C rate and an extremely low capacity decay rate of 0.018% per cycle after 550 cycles at 2 C rate, outperforming most of the reported cathode materials. Density functional theory calculations suggest that the Mo-N-2/C sites can bifunctionally lower the activation energy for Li2S4 to Li2S conversion and the decomposition barrier of Li2S, accounting for its inherently high activity toward LiPS transformation.
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