4.6 Article

Stack Pressure Measurements to Probe the Evolution of the Lithium-Solid-State Electrolyte Interface

Journal

ACS ENERGY LETTERS
Volume 6, Issue 9, Pages 3261-3269

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c01395

Keywords

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Funding

  1. National Science Foundation [ECCS-2025462, DMR-1652471]
  2. Sloan Research Fellowship in Chemistry from the Alfred P. Sloan Foundation
  3. NASA Space Technology Research Fellowship
  4. Ministry of Trade, Industry & Energy/Korea Institute of Energy Technology Evaluation and Planning (MOTIE/KETEP) [20194010000100]
  5. Korea Evaluation Institute of Industrial Technology (KEIT) [20194010000100] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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Real-time measurement of stack pressure in solid-state batteries provides new insights into the interfacial behavior of solid-state electrolytes, aiding in the understanding of different degradation mechanisms and reaction phenomena. Tracking stack pressure coupled with impedance can distinguish between various phenomena and degradation mechanisms within cells, demonstrating the utility of these electro-chemo-mechanical measurements in understanding solid-state battery behavior.
Although solid-state batteries with lithium metal could enable higher energy density and better safety characteristics than Li-ion batteries, the complex electro-chemo-mechanical evolution of the Li-solid-state electrolyte interface can diminish performance. Here, we measure the stack pressure in real time to provide new insights into the effects of applied stack pressure and electrolyte processing on the interfacial behavior of two representative solid-state electrolytes, Li10SnP2S12 and Li6PS5Cl; these materials exhibit different degradation mechanisms through either interphase formation or Li filament growth. We find that stack pressure evolution sensitively depends on interphase formation and that tracking stack pressure coupled with impedance can distinguish between various reaction phenomena and degradation mechanisms within cells. Furthermore, Li filament growth exhibits distinct stack pressure signatures that depend on electrolyte density. The findings advance our understanding of the interfacial evolution of two important classes of solid-state electrolytes, and they demonstrate the utility of electro-chemo-mechanical measurements to understand solid-state battery behavior.

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