How Particle Size Affects Consolidation Behavior, Strain and Properties of Li <sub>6</sub> PS <sub>5</sub> Cl Fast Ionic Conductors

ABSTRACT Solid‐state battery fabrication requires the densification of solid electrolytes to achieve optimal cycling performance and high energy density. However, the underlying compaction mechanisms of these electrolytes remain poorly understood. Here, we investigate the effect of pressure consolidation on the ionic conductor Li 6 PS 5 Cl with particle size distributions (PSD) ranging from 4 to 40 µm. Heckel analysis reveals that samples with smaller PSDs exhibit higher compressibility at lower pressures. X‐ray diffraction peak profiling shows that applied pressure induces lattice strain, leading to peak broadening, while pair distribution function analysis demonstrates a reduction in coherence length upon pressing. Dark‐field X‐ray microscopy further provides spatially resolved orientation maps, uncovering intragranular structural variations within individual Li 6 PS 5 Cl agglomerates after compression. To better understand the origin of stress fluctuations, we performed discrete element method simulations using the experimental PSDs. The results indicate that smaller particles and broader PSDs experience higher stresses, whereas monodisperse systems do not exhibit significant stress fluctuations with position or particle size. This suggests that the high strain observed cannot be attributed solely to smaller particles, but rather to size inhomogeneity. Overall, these findings highlight that both particle size and its distribution play a critical role in processing solid electrolytes for solid‐state batteries.

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Publication Details

Journal
Advanced Energy Materials
Published
2026-01-19
DOI
https://doi.org/10.1002/aenm.202505186
Citations
1
Primary Topic
Advanced Battery Materials and Technologies
Type
article
Field-Weighted Citation Impact
21.93

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How Particle Size Affects Consolidation Behavior, Strain and Properties of Li 6 PS 5 Cl Fast Ionic Conductors

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article

How Particle Size Affects Consolidation Behavior, Strain and Properties of Li 6 PS 5 Cl Fast Ionic Conductors

Dominik Daisenberger, Daniel Rettenwander, Mohammed Alabdali, Can Yıldırım, Wolfgang G. Zeier, Martin Lange, Franco M. Zanotto, Oliver Maus, Vasiliki Faka, Jędrzej Kondek, K. Ganga, Mikael Dahl Kanedal, Matthias Hartmann, Jozef Keckes, Michael Ryan Hansen
article en
1 citations

Abstract

ABSTRACT Solid‐state battery fabrication requires the densification of solid electrolytes to achieve optimal cycling performance and high energy density. However, the underlying compaction mechanisms of these electrolytes remain poorly understood. Here, we investigate the effect of pressure consolidation on the ionic conductor Li 6 PS 5 Cl with particle size distributions (PSD) ranging from 4 to 40 µm. Heckel analysis reveals that samples with smaller PSDs exhibit higher compressibility at lower pressures. X‐ray diffraction peak profiling shows that applied pressure induces lattice strain, leading to peak broadening, while pair distribution function analysis demonstrates a reduction in coherence length upon pressing. Dark‐field X‐ray microscopy further provides spatially resolved orientation maps, uncovering intragranular structural variations within individual Li 6 PS 5 Cl agglomerates after compression. To better understand the origin of stress fluctuations, we performed discrete element method simulations using the experimental PSDs. The results indicate that smaller particles and broader PSDs experience higher stresses, whereas monodisperse systems do not exhibit significant stress fluctuations with position or particle size. This suggests that the high strain observed cannot be attributed solely to smaller particles, but rather to size inhomogeneity. Overall, these findings highlight that both particle size and its distribution play a critical role in processing solid electrolytes for solid‐state batteries.

Advanced Energy MaterialsVol. 16(12)
Centre National de la Recherche Scientifique (FR), AIT Austrian Institute of Technology GmbH (AT), Austrian Academy of Sciences (AT), Montanuniversität Leoben (AT), Institut Universitaire de France (FR), Norwegian University of Science and Technology (NO), University of Münster (DE), European Synchrotron Radiation Facility (FR), Diamond Light Source (GB), Réseau sur le Stockage Electrochimique de l'énergie (FR), Alistore (FR), Laboratoire de Réactivité et Chimie des Solides (FR), Erich Schmid Institute of Materials Science (AT), Helmholtz-Institute Münster (DE)
Österreichische Nationalstiftung für Forschung, Technologie und Entwicklung, Diamond Light Source, European Commission, Agence Nationale de la Recherche, European Synchrotron Radiation Facility, Bundesministerium für Bildung und Forschung, Institut Universitaire de France, Christian Doppler Forschungsgesellschaft, Bundesministerium für Digitalisierung und Wirtschaftsstandort, HORIZON EUROPE Framework Programme
Affordable and clean energy
Openalex Percentile: Top 2%
Advanced Battery Materials and Technologies
21.93
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