Elimination of detrimental grain boundary segregation in Garnets

Abstract Garnet Li 7 La 3 Zr 2 O 12 electrolyte is considered a key enabler of solid-state batteries with Li metal electrodes, but the grain boundaries impair its performance. To date, the understanding of grain boundary structures and its impact on performance remains elusive. Here, we show that element segregation at Li 7 La 3 Zr 2 O 12 grain boundaries critically governs Li transport and nucleation. During conventional sintering, Al, Ta, and La segregate at grain boundaries, locally depleting Li and creating space-charge layers that lower total ionic conductivity. Simultaneously, this segregation leads to higher electronic conductivity along grain boundaries, which promotes Li nucleation at grain boundary edges with increased risk of dendrite formation. The underlying mechanism of segregation is governed by both thermodynamic driving forces and diffusion kinetics. Building on this understanding, we develop a strategy to achieve segregation-free grain boundaries through a rapid sintering protocol that utilizes the onset of solid-state softening. This approach yields transparent, polycrystalline Li 7 La 3 Zr 2 O 12 with negligible grain boundary impedance and enhanced dendrite tolerance. By elucidating the structural origins and electrochemical consequences of grain boundary segregation, this work provides a guidance for the rational optimization of solid electrolytes.

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Publication Details

Journal
Nature Communications
Published
2026-06-29
DOI
https://doi.org/10.1038/s41467-026-74887-z
Primary Topic
Advanced Battery Materials and Technologies
Type
article
Field-Weighted Citation Impact
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article

Elimination of detrimental grain boundary segregation in Garnets

Timo Danner, Brandon C. Wood, Qianli Ma, Walter Sebastian Scheld et al.
Nature Communications
Advanced Battery Materials and Technologies
article

Elimination of detrimental grain boundary segregation in Garnets

Timo Danner, Brandon C. Wood, Qianli Ma, Walter Sebastian Scheld, Arnulf Latz, Olivier Guillon, Johan E. ten Elshof, Kwangnam Kim, Liwen F. Wan, Mark Huijben, Christoph Roitzheim, Jan Dippell, Dina Fattakhova‐Rohlfing, Lei Jin, Yuan Zeng, Dylan Jennings, Kai Yao, Martin Finsterbusch, Xingyu Liu, Meng Ma
article en

Abstract

Abstract Garnet Li 7 La 3 Zr 2 O 12 electrolyte is considered a key enabler of solid-state batteries with Li metal electrodes, but the grain boundaries impair its performance. To date, the understanding of grain boundary structures and its impact on performance remains elusive. Here, we show that element segregation at Li 7 La 3 Zr 2 O 12 grain boundaries critically governs Li transport and nucleation. During conventional sintering, Al, Ta, and La segregate at grain boundaries, locally depleting Li and creating space-charge layers that lower total ionic conductivity. Simultaneously, this segregation leads to higher electronic conductivity along grain boundaries, which promotes Li nucleation at grain boundary edges with increased risk of dendrite formation. The underlying mechanism of segregation is governed by both thermodynamic driving forces and diffusion kinetics. Building on this understanding, we develop a strategy to achieve segregation-free grain boundaries through a rapid sintering protocol that utilizes the onset of solid-state softening. This approach yields transparent, polycrystalline Li 7 La 3 Zr 2 O 12 with negligible grain boundary impedance and enhanced dendrite tolerance. By elucidating the structural origins and electrochemical consequences of grain boundary segregation, this work provides a guidance for the rational optimization of solid electrolytes.

Nature Communications
Lawrence Livermore National Laboratory (US), Northwestern Polytechnical University (CN), Forschungszentrum Jülich (DE), Universität Ulm (DE), Ernst Ruska Centre (DE), Deutsches Zentrum für Luft- und Raumfahrt e. V. (DLR) (DE), Helmholtz-Institute Ulm (DE), Helmholtz-Institute Münster (DE), Jülich Aachen Research Alliance (DE), Lawrence Livermore National Security (US), University of Duisburg-Essen (DE), Ruhr University Bochum (DE), University of Twente (NL)
Openalex Percentile: Top 12%
Advanced Battery Materials and Technologies
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