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Impact of the Chlorination of Lithium Argyrodites on the Electrolyte/Cathode Interface in Solid-State Batteries |
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| Authors: | Dr Tong-Tong Zuo Dr Felix Walther Jun Hao Teo Dr Raffael Rueß Yubo Wang Prof Marcus Rohnke Prof Daniel Schröder Prof Linda F Nazar Prof Jürgen Janek |
| Institution: | 1. Institute of Physical Chemistry, Justus Liebig University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany;2. Institute of Physical Chemistry, Justus Liebig University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany
Center for Materials Research (ZfM/LaMa), Justus Liebig University Giessen, Heinrich-Buff-Ring 16, 35392 Giessen, Germany;3. Battery and Electrochemistry Laboratory, Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany;4. Department of Chemistry and the Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue West, Waterloo, Ontario N2L 3G1 Canada;5. Institute of Energy and Process Systems Engineering (InES), Technische Universität Braunschweig, Langer Kamp 19B, 38106 Braunschweig, Germany |
| Abstract: | Lithium argyrodite-type electrolytes are regarded as promising electrolytes due to their high ionic conductivity and good processability. Chemical modifications to increase ionic conductivity have already been demonstrated, but the influence of these modifications on interfacial stability remains so far unknown. In this work, we study Li6PS5Cl and Li5.5PS4.5Cl1.5 to investigate the influence of halogenation on the electrochemical decomposition of the solid electrolyte and the chemical degradation mechanism at the cathode interface in depth. Electrochemical measurements, gas analysis and time-of-flight secondary ion mass spectrometry indicate that the Li5.5PS4.5Cl1.5 shows pronounced electrochemical decomposition at lower potentials. The chemical reaction at higher voltages leads to more gaseous degradation products, but a lower fraction of solid oxygenated phosphorous and sulfur species. This in turn leads to a decreased interfacial resistance and thus a higher cell performance. |
| Keywords: | Composite Cathode Interfacial Stability Lithium Argyrodite Electrolyte Solid State Battery |