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REVIEWS Understanding interface stability in solid-state batteries Yihan Xiao 1,2, Yan Wang 3, Shou-Hang Bo 2,4, Jae Chul Kim 2,5, Lincoln J. Miara3 and Gerbrand Ceder 1,2* 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. 1Department of Materials Science and Engineering, University of California Berkeley, Berkeley, CA, USA. 2Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. 3Advanced Materials Lab, Samsung Research America, Burlington, MA, USA. 4University of Michigan– Shanghai Jiao Tong University Joint Institute, Shanghai Jiao Tong University, Shanghai, China. 5Department of Chemical Engineering and Materials Science, Stevens Institute of Technology, Hoboken, NJ, USA. *e-mail: gceder@ berkeley.edu https://doi.org/10.1038/ s41578-019-0157-5 Rechargeable Li-ion batteries have revolutionized the energy-storage market and enabled the widespread use of portable electronic devices and electric vehicles. Replacing the liquid electrolyte in conventional Li-ion batteries with a solid electrolyte (SE) can further improve their energy densities and safety by reducing flammability, improving the cycle life and enabling the use of alkali-metal anodes. Unlike currently used organic liquid electrolytes, inor- ganic solid-state conductors are non-flammable or have much higher onset temperatures for thermal runaway. The reactivity of liquid electrolytes with electrodes also contributes substantially to the capacity fade of the bat- tery1,2. Such electrolyte decomposition can, in principle, be mitigated by selecting an inorganic material that is thermodynamically stable or can passivate further reac- tions with electrodes. Indeed, minimal capacity fade over 10,000 cycles was observed in a solid-state cell employing a thin-film lithium phosphorus oxynitride (LiPON) elec- trolyte3. SEs may also enable the use of lithium or sodium metal anodes, which have much higher volumetric and gravimetric capacities than graphite or hard carbon4,5. In liquid electrolytes, the formation of metal dendrites can short-circuit the cell6,7. By contrast, some SEs have shown potential to suppress dendrite formation3,8,9, but the general effectiveness of ceramics in preventing dendrite growth between the electrodes remains in question10,11. The development of solid-state batteries (SSBs) has, in part, been limited by the lack of solid materials with room-temperature ionic conductivities comparable to those of liquid electrolytes. However, this issue has been overcome in the past 15 years. The room-temperature conductivity of LiPF6 and NaPF6 in the liquid solvent ethylene carbonate:dimethyl carbonate (EC:DMC) is 5–10 mS cm−1 (refs12,13). Several SEs have been reported that exhibit a ionic conductivity comparable or higher than that of liquid electrolytes, with a Li-ion transference number close to 1 (compared with values often below 0.5 in liquid electrolytes)13. These superionic conductors include the Na superionic conductor (NASICON)-type oxides14–19, Li and Na β-alumina20–23, Li garnets24–27, perovskites28 and antiperovskites29. Sulfides, including thio-Li superionic conductor (LISICON)-type com- pounds Li M P S (M=Ge, Si)30,31, Li GeP S (LGPS)32 4−x 1−x x 4 10 2 12 and its derivatives33,34, Li2S–P2S5 glass35 and Li7P3S11 glass-ceramic36, and argyrodites Li6PS5X (X = Cl, Br, I)37,38, constitute another large family of superionic conductors. To date, the highest room-temperature Li-ion conductivity reported in an SE is 25 mS cm−1 in LGPS-type Li9.54Si1.74P1.44S11.7Cl0.3 (ref.33). High ionic con- ductivity has also been achieved in Na-ion sulfides such as Na PS (refs39,40), Na PSe (ref.41), Na SbS (ref.42) and 343434 Na10SnP2S12 (refs43,44), as well as in alkali closo-borates45,46. Nature reviews | MaterialsPDF Image | Understanding interface stability in solid-state batteries
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