Abstract

A common practise in the research of Li–S batteries is to use high electrode porosity and excessive electrolytes to boost sulfur-specific capacity. Here we propose a class of dense intercalation-conversion hybrid cathodes by combining intercalation-type Mo6S8 with conversion-type sulfur to realize a Li–S full cell. The mechanically hard Mo6S8 with fast Li-ion transport ability, high electronic conductivity, active capacity contribution and high affinity for lithium polysulfides is shown to be an ideal backbone to immobilize the sulfur species and unlock their high gravimetric capacity. Cycling stability and rate capability are reported under realistic conditions of low carbon content (~10 wt%), low electrolyte/active material ratio (~1.2 µl mg−1), low cathode porosity (~55 vol%) and high mass loading (>10 mg cm−2). A pouch cell assembled based on the hybrid cathode and a 2× excess Li metal anode is able to simultaneously deliver a gravimetric energy density of 366 Wh kg−1 and a volumetric energy density of 581 Wh l−1.

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Acknowledgements

We acknowledge the support by Samsung Advanced Institute of Technology, National Key Technologies R&D Program, China (grant no. 2018YFB0104400) and the National Natural Science Foundation of China (grant no. 51872322). We also acknowledge the valuable suggestions for experiments from L. Miao and the carbonaceous materials provided by B. Fugetsu at School of Engineering, The University of Tokyo. This work made use of the MRSEC Shared Experimental Facilities supported by the National Science Foundation under award no. DMR-1419807. L.S. acknowledges the One Hundred Talent Project of the Chinese Academy of Sciences and Thousand Talents Program for Young Scientists.

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Affiliations

  1. Department of Nuclear Science and Engineering and Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    • Weijiang Xue
    • , Zhe Shi
    • , Liumin Suo
    • , Chao Wang
    • , Ziqiang Wang
    • , Kang Pyo So
    • , Yuming Chen
    • , Long Qie
    • , Zhi Zhu
    • , Guiyin Xu
    •  & Ju Li
  2. Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China

    • Liumin Suo
  3. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, China

    • Liumin Suo
  4. Songshan Lake Materials Laboratory, Dongguan, Guangdong, China

    • Liumin Suo
  5. Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, USA

    • Haozhe Wang
    • , Daiwei Yu
    •  & Jing Kong
  6. Advanced Materials Lab , Samsung Advanced Institute of Technology America, Burlington, MA, USA

    • Andrea Maurano
  7. Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai, China

    • Long Qie

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Contributions

L.S., W.X. and J.L. conceived and designed the experiments. W.X., L.S. and C.W. fabricated the HMSC cathode. W.X., K.P.S., Y.C., L.Q., Z.Z. and G.X. carried out material characterization and electrochemical measurements. Z.S. carried out the DFT theoretical calculations. Z.W. and D.Y. carried out the TEM observation. H.W. and J.K. conducted the four-point-probe resistivity test. W.X., C.W. and A.M. made the pouch cell. W.X., L.S., J.L. and Z.S. wrote the paper. All authors discussed the results and reviewed the manuscript.

Competing interests

The authors declare no competing interests.

Corresponding authors

Correspondence to Liumin Suo or Ju Li.

Supplementary information

  1. Supplementary Information

    Supplementary Figures 1–25, Supplementary Note 1, Supplementary Tables 1–3.

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DOI

https://doi.org/10.1038/s41560-019-0351-0