Evolving contact mechanics and microstructure formation dynamics of the lithium metal-Li7La3Zr2O12 interface

Wesley Chang, Richard May, Michael Wang, Gunnar Thorsteinsson, Jeff Sakamoto, Lauren Marbella () and Daniel Steingart ()
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Wesley Chang: Princeton University
Richard May: Columbia University
Michael Wang: University of Michigan
Gunnar Thorsteinsson: Columbia University
Jeff Sakamoto: University of Michigan
Lauren Marbella: Columbia University
Daniel Steingart: Columbia University

Nature Communications, 2021, vol. 12, issue 1, 1-12

Abstract: Abstract The dynamic behavior of the interface between the lithium metal electrode and a solid-state electrolyte plays a critical role in all-solid-state battery performance. The evolution of this interface throughout cycling involves multiscale mechanical and chemical heterogeneity at the micro- and nano-scale. These features are dependent on operating conditions such as current density and stack pressure. Here we report the coupling of operando acoustic transmission measurements with nuclear magnetic resonance spectroscopy and magnetic resonance imaging to correlate changes in interfacial mechanics (such as contact loss and crack formation) with the growth of lithium microstructures during cell cycling. Together, the techniques reveal the chemo-mechanical behavior that governs lithium metal and Li7La3Zr2O12 interfacial dynamics at various stack pressure regimes and with voltage polarization.

Date: 2021
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DOI: 10.1038/s41467-021-26632-x

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