Publication date: 10th April 2024
Although solid-state batteries with metal anodes promise to enable safer, higher energy density batteries, metal protrusions (dendrites) grow when charging faster than a critical current density.1,2 It is generally believed that dendrites grow when plating-induced stresses exceed that required for fracture of the solid-electrolyte.2–4 It is commonly assumed that the threshold stress for failure depends on the electrolyte's fracture toughness—commonly taken as a material constant.2–4 Here we use operando birefringence microscopy5 to directly measure dendrite-induced stresses. We find that increasing current densities increase the dendrite velocity. Dendrite-induced stresses appear to evolve with time—even during dendrite propagation—in a fashion that depends on the current density or dendrite velocity. Cryogenic Scanning Transmission Electron Microscopy (Cryo-STEM) reveals decomposed electrolyte phases at the dendrite tip. This decomposition is associated with a volume contraction. All experiments were conducted on the most electrochemically stable Li-ion conducting solid electrolyte (tantalum-doped lithium lanthanum zirconium oxide).6 Together, these experiments allow separate study of electrochemical and mechanical phenomena underlying dendrite growth in ceramic electrolytes.
References
1. Sudworth, J. L., Hames, M. D., Storey, M. A., Azim, M. F. & Tilley, A. R. An analysis and laboratory assessment of Two Sodium Sulfur Cell Designs. Power Sources 4, 1–18 (1972).
2. Sharafi, A., Meyer, H. M., Nanda, J., Wolfenstine, J. & Sakamoto, J. Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density. J. Power Sources 302, 135–139 (2016).
3. Fincher, C. D. et al. Controlling dendrite propagation in solid-state batteries with engineered stress. Joule 6, 2794-2809 (2022).
4. Porz, L. et al. Mechanism of lithium metal penetration through inorganic solid electrolytes. Adv. Energy Mater. 7, 1701003 (2017).
5. Athanasiou†, C. E., Fincher†, C. D. et al. Operando measurements of dendrite-induced stresses in ceramic electrolytes using photoelasticity. Matter (2023).
Funding is gratefully acknowledged from Mechano-Chemical Understanding of Solid Ion Conductors, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, contract DE-SC0023438C. B.W.S. acknowledges funding from NSF (DMR-2124775). C. F. acknowledges funding from the Department of Defense National Defense Science and Engineering Graduate Fellowship.
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