Understanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques

Chao Zhu, Till Fuchs, Stefan A. L. Weber, Felix. H. Richter, Gunnar Glasser, Franjo Weber, Hans-Jürgen Butt, Jürgen Janek () and Rüdiger Berger ()
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Chao Zhu: Max Planck Institute for Polymer Research
Till Fuchs: Institute of Physical Chemistry & Center for Materials Research, Justus Liebig University Giessen
Stefan A. L. Weber: Max Planck Institute for Polymer Research
Felix. H. Richter: Institute of Physical Chemistry & Center for Materials Research, Justus Liebig University Giessen
Gunnar Glasser: Max Planck Institute for Polymer Research
Franjo Weber: Max Planck Institute for Polymer Research
Hans-Jürgen Butt: Max Planck Institute for Polymer Research
Jürgen Janek: Institute of Physical Chemistry & Center for Materials Research, Justus Liebig University Giessen
Rüdiger Berger: Max Planck Institute for Polymer Research

Nature Communications, 2023, vol. 14, issue 1, 1-14

Abstract: Abstract The growth of lithium dendrites in inorganic solid electrolytes is an essential drawback that hinders the development of reliable all-solid-state lithium metal batteries. Generally, ex situ post mortem measurements of battery components show the presence of lithium dendrites at the grain boundaries of the solid electrolyte. However, the role of grain boundaries in the nucleation and dendritic growth of metallic lithium is not yet fully understood. Here, to shed light on these crucial aspects, we report the use of operando Kelvin probe force microscopy measurements to map locally time-dependent electric potential changes in the Li6.25Al0.25La3Zr2O12 garnet-type solid electrolyte. We find that the Galvani potential drops at grain boundaries near the lithium metal electrode during plating as a response to the preferential accumulation of electrons. Time-resolved electrostatic force microscopy measurements and quantitative analyses of lithium metal formed at the grain boundaries under electron beam irradiation support this finding. Based on these results, we propose a mechanistic model to explain the preferential growth of lithium dendrites at grain boundaries and their penetration in inorganic solid electrolytes.

Date: 2023
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DOI: 10.1038/s41467-023-36792-7

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