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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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.
The authors declare no competing interests.
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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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