Intercalation-conversion hybrid cathodes enabling Li–S full-cell architectures with jointly superior gravimetric and volumetric energy densities

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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Fig. 1: Design strategy for jointly high gravimetric–volumetric energy density.
Fig. 2: Characterizations of the HMSC and traditional C/S8 cathode.
Fig. 3: Investigation of the interaction between LixMo6S8 and LiPS.
Fig. 4: The roles of the Chevrel-phase Mo6S8 in the HMSC.
Fig. 5: Electrochemical performance of the Li|HMSC coin cell.
Fig. 6: The Eg and Ev of the Li|HMSC cell.

Data availability

The data that support the plots in this paper and other findings of this study are available from the corresponding author on reasonable request.

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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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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.

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Correspondence to Liumin Suo or Ju Li.

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

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Xue, W., Shi, Z., Suo, L. et al. Intercalation-conversion hybrid cathodes enabling Li–S full-cell architectures with jointly superior gravimetric and volumetric energy densities. Nat Energy 4, 374–382 (2019). https://doi.org/10.1038/s41560-019-0351-0

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