Study of structural and electrochemical evolution of LPSCL during “cold sintering” process

Ove Korjus^a^,^b, Saptarshee Mitra^b, Quentin Berrod^a^,^b, Victor Vanpeene^a, Markus Appel^a, Emanuelle Suard^a, Sandrine Lyonnard^b, Claire Villevieille^c

^aInstitut Laue-Langevin - 71 avenue des Martyrs CS 20156, 38042 GRENOBLE Cedex

^bCEA Grenoble, 17 rue des Martyrs, Grenoble, France

^cUniv. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP*, LEPMI, 38000 Grenoble, France

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

Advanced characterisation techniques: fundamental and devices

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

Organizers: John Kilner and Stephen Skinner

Poster, Ove Korjus, 623
Publication date: 10th April 2024

Solid-state lithium-ion batteries (SLIBs) are envisaged as next-generation to conventional Li-ion batteries. However, to date, they have suffered several issues arising from the engineering and control of their solid-solid interfaces.

Li₆PS₅Cl (LPSCL), one material from the thiophosphate family, possesses several advantages, such as high ionic conductivity and a “cold sintered” ability¹. However, the ionic conductivity can range from 0.06 mS.cm^-¹ to 4.73 mS.cm^-¹ at room temperature^2,3 based on materials quality, granulometry surface chemistry, etc., which explains such an extensive results dispersion.

In this study, we conducted in situ “cold sintering” of Li₆PS₅Cl electrolyte while simultaneously measuring Electrochemical Impedance Spectroscopy and micro X-ray tomography at ID19 in the European Synchrotron Radiation Facility (ESRF) to understand the “cold sintering” process of LPSCL electrolyte and establish the relationship between tortuosity, electrolyte microstructure and ionic conductivities.

One of the things we saw from the in situ “cold sintering” experiment was the intense cracking of big LPSCL secondary particles (Fig. 2a.), and at the same time, not many changes to the particle shape of the secondary particles. We saw an evolution of electrolyte conductivity from the simultaneous electrochemical impedance spectroscopy measurements (Fig. 2b.). To get more information about the nature of the conductivity change during the “cold sintering” of the electrolyte, additional advanced laboratory experiments using electrochemical impedance spectroscopy at very low temperatures were carried out. It helped us to separate the grain boundaries evolution to one of the bulk ionic conductivity, giving a new correlation between electrode microstructure and electrochemical measurement.

References:

[1] Mangani, L. R. & Villevieille, C. Mechanical vs. chemical stability of sulphide-based solid-state batteries. Which one is the biggest challenge to tackle? Overview of solid-state batteries and hybrid solid state batteries. J. Mater. Chem. A 8, 10150–10167 (2020)

[2] Rosero-Navarro, N. C., Miura, A. & Tadanaga, K. Preparation of lithium ion conductive Li6PS5Cl solid electrolyte from solution for the fabrication of composite cathode of all-solid-state lithium battery. J. Sol-Gel Sci. Technol. 89, 303–309 (2019)

[3] Yu, C. et al. Facile Synthesis toward the Optimal Structure-Conductivity Characteristics of the Argyrodite Li6PS5Cl Solid-State Electrolyte. ACS Appl. Mater. Interfaces 10, 33296–33306 (2018)

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