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A high-energy and long-cycling lithium–sulfur pouch cell via a macroporous catalytic cathode with double-end binding sites

Nature Nanotechnology volume 16, pages 166–173 (2021)Cite this article

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An Author Correction to this article was published on 03 December 2020

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Abstract

Lithium–sulfur batteries are attractive alternatives to lithium-ion batteries because of their high theoretical specific energy and natural abundance of sulfur. However, the practical specific energy and cycle life of Li–S pouch cells are significantly limited by the use of thin sulfur electrodes, flooded electrolytes and Li metal degradation. Here we propose a cathode design concept to achieve good Li–S pouch cell performances. The cathode is composed of uniformly embedded ZnS nanoparticles and Co–N–C single-atom catalyst to form double-end binding sites inside a highly oriented macroporous host, which can effectively immobilize and catalytically convert polysulfide intermediates during cycling, thus eliminating the shuttle effect and lithium metal corrosion. The ordered macropores enhance ionic transport under high sulfur loading by forming sufficient triple-phase boundaries between catalyst, conductive support and electrolyte. This design prevents the formation of inactive sulfur (dead sulfur). Our cathode structure shows improved performances in a pouch cell configuration under high sulfur loading and lean electrolyte operation. A 1-A-h-level pouch cell with only 100% lithium excess can deliver a cell specific energy of >300 W h kg−1 with a Coulombic efficiency >95% for 80 cycles.

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Fig. 1: Design strategy of macroporous host with DEB sites.
Fig. 2: Structure characterizations of macroporous host with DEB sites.
Fig. 3: Density functional theory calculations.
Fig. 4: Coin-cell characterization.
Fig. 5: Phase transformation and interphase characterization.
Fig. 6: Pouch-cell characterization.

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Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

Research at the Argonne National Laboratory was funded by the US Department of Energy (DOE), Vehicle Technologies Office. Support from T. Duong of the US DOE’s Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source, an Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory, was supported by DOE under contract no. DE-AC02-06CH11357. This work was also supported by a grant from the Research Grants Council of the Hong Kong Special Administrative Region, China (project no. T23-601/17-R). K.A. and G.X. also thank the support from Clean Vehicles, US-China Clean Energy Research Centre (CERC-CVC2). K.A. and G.-L.X. thank S. Ahmed at Argonne National Laboratory for the simulation on the cell specific energy of Li–S and NMC811–graphite pouch cells.

Author information

Authors and Affiliations

  1. Department of Mechanical and Aerospace Engineering, Hong Kong University of Science and Technology, Hong Kong, China

    Chen Zhao, Leicheng Zhang, Yuxun Ren & Tianshou Zhao

  2. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA

    Chen Zhao, Gui-Liang Xu & Khalil Amine

  3. Materials Science Division, Argonne National Laboratory, Lemont, IL, USA

    Zhou Yu & Lei Cheng

  4. X-ray Science Division, Argonne National Laboratory, Lemont, IL, USA

    Inhui Hwang, Cheng-Jun Sun, Yang Ren & Xiaobing Zuo

  5. Collaborative Innovation Centre of Chemistry for Energy Materials, State Key Laboratory Physical Chemistry of Solid Surfaces, Department of Chemistry, Xiamen University, Xiamen, China

    Yu-Xue Mo & Shi-Gang Sun

  6. College of Energy, Xiamen University, Xiamen, China

    Jun-Tao Li

  7. Materials Science and Engineering, Stanford University, Stanford, CA, USA

    Khalil Amine

  8. Institute for Research & Medical Consultations, Imam Abdulrahman Bin Faisal University (IAU), Dammam, Saudi Arabia

    Khalil Amine

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Contributions

G.-L.X., K.A. and T.Z. initiated this research project. G.-L.X. conceived the idea and designed the experiment under the supervision of K.A. and T.Z.; C.Z. synthesized and characterized the structures of the materials and tested the half-cells and pouch cells with the assistance of L.Z. and Yuxun Ren; G.-L.X., I.H., C.-J.S., Yang Ren and X.Z. conducted synchrotron X-ray measurements and analysis. Z.Y. and L.C. conducted the calculation simulation. Y.-X.M., J.-T.L. and S.-G.S. conducted the in situ UV-vis measurement. C.Z., G.-L.X., K.A. and T.Z. prepared the manuscript. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Gui-Liang Xu, Khalil Amine or Tianshou Zhao.

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Peer review information Nature Nanotechnology thanks Long Qie, Yunxiao Wang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–33, Materials and Methods, Discussion, Tables 1–6 and refs. 1–75.

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Zhao, C., Xu, GL., Yu, Z. et al. A high-energy and long-cycling lithium–sulfur pouch cell via a macroporous catalytic cathode with double-end binding sites. Nat. Nanotechnol. 16, 166–173 (2021). https://doi.org/10.1038/s41565-020-00797-w

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