4.8 Article

Precise Synthesis of Fe-N2 Sites with High Activity and Stability for Long-Life Lithium-Sulfur Batteries

Journal

ACS NANO
Volume 14, Issue 11, Pages 16105-16113

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c08056

Keywords

lithium-sulfur batteries; Fe-NC catalyst; Fe-N-2 sites; sulfur reduction reaction; polysulfides; shuttle effect

Funding

  1. National Natural Science Foundation of China [21646012]
  2. China Postdoctoral Science Foundation [2016M600253, 2017T100246]
  3. Postdoctoral Foundation of Heilongjiang Province [LBH-Z16060]

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Precisely tuning the coordination environment of the metal center and further maximizing the activity of transition metal-nitrogen carbon (M-NC) catalysts for high-performance lithium-sulfur batteries are greatly desired. Herein, we construct an Fe-NC material with uniform and stable Fe-N-2 coordination structure. The theoretical and experimental results indicate that the unsaturated Fe-N-2 center can act as a multifunctional site for anchoring lithium polysulfides (LiPSs), accelerating the redox conversion of LiPSs and reducing the reaction energy barrier of Li2S decomposition. Consequently, the batteries based on a porous carbon nitride supported Fe-N-2 site (Fe-N-2/CN) host exhibit excellent cycling performance with a capacity decay of 0.011% per cycle at 2 C after 2000 cycles. This work deepens the understanding of the relationship between electronic structure of M-NC sites and the catalysis effect for the conversion of LiPSs. This strategy also provides a potent guidance for the further application of M-NC materials in advanced lithium-sulfur batteries.

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