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Understanding interface stability in solid-state batteries

Nature Reviews Materials volume 5, pages 105–126 (2020)Cite this article

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A Publisher Correction to this article was published on 09 March 2020

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Abstract

Solid-state batteries (SSBs) using a solid electrolyte show potential for providing improved safety as well as higher energy and power density compared with conventional Li-ion batteries. However, two critical bottlenecks remain: the development of solid electrolytes with ionic conductivities comparable to or higher than those of conventional liquid electrolytes and the creation of stable interfaces between SSB components, including the active material, solid electrolyte and conductive additives. Although the first goal has been achieved in several solid ionic conductors, the high impedance at various solid/solid interfaces remains a challenge. Recently, computational models based on ab initio calculations have successfully predicted the stability of solid electrolytes in various systems. In addition, a large amount of experimental data has been accumulated for different interfaces in SSBs. In this Review, we summarize the experimental findings for various classes of solid electrolytes and relate them to computational predictions, with the aim of providing a deeper understanding of the interfacial reactions and insight for the future design and engineering of interfaces in SSBs. We find that, in general, the electrochemical stability and interfacial reaction products can be captured with a small set of chemical and physical principles.

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Fig. 1: Interfaces in cathode composites.
Fig. 2: Interface models for the evaluation of (electro)chemical stability.
Fig. 3: (Electro)chemical instability of sulfide solid electrolytes.
Fig. 4: (Electro)chemical instability of garnet solid electrolytes.
Fig. 5: Polyanionic oxides as a bridge between oxides and sulfides for good chemical compatibility.
Fig. 6: Electrochemical stability windows of common solid electrolytes.
Fig. 7: Trade-offs between ionic conductivity and electrochemical stability upon tuning the solid electrolyte composition.

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Acknowledgements

The work on ionic conductivity design was funded by the Samsung Advanced Institute of Technology. The development of the interfacial reactivity theory was funded by the Materials Project Program (grant no. KC23MP) through the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract no. DE-AC02-05CH11231. Some of the work on sulfide electrolytes was supported by the Assistant Secretary of Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the U.S. Department of Energy under contract no. DE-AC02-05CH11231 under the Advanced Battery Materials Research (BMR) Program.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, University of California Berkeley, Berkeley, CA, USA

    Yihan Xiao & Gerbrand Ceder

  2. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Yihan Xiao, Shou-Hang Bo, Jae Chul Kim & Gerbrand Ceder

  3. Advanced Materials Lab, Samsung Research America, Burlington, MA, USA

    Yan Wang & Lincoln J. Miara

  4. University of Michigan–Shanghai Jiao Tong University Joint Institute, Shanghai Jiao Tong University, Shanghai, China

    Shou-Hang Bo

  5. Department of Chemical Engineering and Materials Science, Stevens Institute of Technology, Hoboken, NJ, USA

    Jae Chul Kim

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  1. Yihan Xiao
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Contributions

G.C. conceived the manuscript. Y.X. researched the data. S.-H.B. and Y.X. wrote the section on sulfides. Y.X. wrote the sections on garnets and coatings. J.C.K. wrote the sections on LiPON and antiperovskites. Y.W. and Y.X. wrote the sections on perovskites and NASICONs. G.C., Y.X. and L.J.M. wrote the discussion and conclusions sections. Y.X., Y.W. and L.J.M. designed the table and figures. All authors edited and reviewed the manuscript before submission.

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Correspondence to Gerbrand Ceder.

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Xiao, Y., Wang, Y., Bo, SH. et al. Understanding interface stability in solid-state batteries. Nat Rev Mater 5, 105–126 (2020). https://doi.org/10.1038/s41578-019-0157-5

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