Engineering high conductive percolating networks in Li6PS5Cl tapes for solid-state batteries.

Quoc-Anh Tran^a^,^b, Meenal Agrawal^a^,^b, Michael Häusler^d, Juraj Todt^e^,^f, Laras Fadillah^a, Mir Mehraj Ud Din^a^,^b, Roman Zettl^c, Volker Henninge^c, Jozef Keckes^e^,^f, Roland Brunner^d, Per Erik Vullum^g, Daniel Rettenwander^a^,^b

^aDepartment of Materials Science and Engineering, NTNU Norwegian University of Science and Technology, Trondheim, Norway

^bInternational Christian Doppler Laboratory for Solid-State Batteries, NTNU Norwegian University of Science and Technology, Trondheim, Norway

^cAVL List GmbH, Graz, Austria

^dMaterials Center Leoben, Leoben, Austria

^eDepartment of Materials Physics, Montanuniversität Leoben, Leoben, Austria

^fErich Schmid Institute for Materials Science, Austrian Academy of Sciences, Leoben, Austria

^gMaterials and nanotechnology, SINTEF Industry, Trondheim, Norway

Proceedings of 24th International Conference on Solid State Ionics (SSI24)

Emerging Materials for High-Performance Devices

London, United Kingdom, 2024 July 14th - 19th

Organizers: John Kilner and Stephen Skinner

Poster, Quoc-Anh Tran, 606
Publication date: 10th April 2024

Solid-state batteries have emerged as a promising battery technology for the future, offering solutions to common issues associated with Li-ion batteries, particularly safety concerns related to the flammable nature of liquid electrolytes. Furthermore, solid-state batteries hold the potential for higher volumetric and gravimetric energy densities compared to Li-ion batteries₁. Despite considerable advancements in solid-state battery development, the transition from successful lab-scale cells to commercially viable pouch cells remain a significant bottleneck in their commercialization journey, particularly when utilizing inorganic solid electrolytes_2,3.

As a result, significant efforts have been directed towards developing large-scale synthesis techniques for Li₆PS₅Cl solid electrolyte, resulting in the emergence of commercial availability. However, in contrast to small-scale laboratory synthesis, commercial Li₆PS₅Cl production frequently results in a diverse array of particle sizes and distributions, which leads to significant challenges such as low-quality percolation network. In some cases, these challenges extend to the inclusion of particles larger than the composite cathode thickness when integrated into solid-state batteries, exacerbating difficulties related to achieving proper densification and resulting in suboptimal kinetics. Hence, further research is needed to elucidate how microstructural features such as the average particle size and distribution of Li₆PS₅Cl powder effects the electrochemical performance of slurry based casted Li₆PS₅Cl tapes and how the compact grain size and distribution, and solid electrolyte compact pore size and distribution would impact electrochemical performance.

This study delves into optimizing argyrodite Li₆PS₅Cl particle size distribution while maintaining good Li-ion conductivity and subsequently improving the densification of slurry-based casted Li₆PS₅Cl tape. It investigates how the particle size distribution of Li₆PS₅Cl and pre-pressing conditions influence the percolating network. A range of characterization tools, including FIB-SEM, TEM, X-ray computed tomography, and temperature and pressure-dependent impedance spectroscopy, are utilized to establish connections between microstructure and Li-ion transport.

References:

[1] Janek, J. & Zeier, W. G. A solid future for battery development. Nat Energy 1, (2016).

[2] Wang, C., Kim, J. T., Wang, C. & Sun, X. Progress and Prospects of Inorganic Solid‐State Electrolyte‐Based All‐Solid‐State Pouch Cells. Advanced Materials 35, (2023).

[3] Wang, C. et al. All-solid-state lithium batteries enabled by sulfide electrolytes: From fundamental research to practical engineering design. Energy and Environmental Science vol. 14 2577–2619, (202)

Acknowledgements:

We acknowledge financial support by Austrian Federal Ministry for Digital and Economic Affairs, the National Foundation for Research, Technology and Development and the Christian Doppler Research Association (Christian Doppler Laboratory for Solid-State Batteries)

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