Working Principle of an Ionic Liquid Interlayer During Pressureless Lithium Stripping on Li 6.25 Al 0.25 La 3 Zr 2 O 12 (LLZO) Garnet‐Type Solid Electrolyte

Fuchs, Till; Mogwitz, Boris; Otto, Svenja‐Katharina; Passerini, Stefano; Richter, Felix H.; Janek, Jürgen

doi:10.1002/batt.202100015

Working Principle of an Ionic Liquid Interlayer During Pressureless Lithium Stripping on Li _6.25 Al _0.25 La ₃ Zr ₂ O ₁₂ (LLZO) Garnet‐Type Solid Electrolyte

Journal Article · Fri Mar 26 00:00:00 EDT 2021 · Batteries & Supercaps

DOI:https://doi.org/10.1002/batt.202100015· OSTI ID:1772837

Fuchs, Till ^[1]; Mogwitz, Boris ^[1]; Otto, Svenja‐Katharina ^[2]; Passerini, Stefano ^[3]; Richter, Felix H. ^[1]; ^[1]

Institute of Physical Chemistry Justus-Liebig-University Giessen Heinrich-Buff-Ring 17 35392 Giessen Germany, Center for Materials Research (ZfM) Justus-Liebig-University Giessen Heinrich-Buff-Ring 16 35392 Giessen Germany
Institute of Physical Chemistry Justus-Liebig-University Giessen Heinrich-Buff-Ring 17 35392 Giessen Germany
Helmholtz Institute Ulm Helmholtzstraße 11 89081 Ulm Germany, Karlsruhe Institute of Technology (KIT) P.O. Box 3640 76021 Karlsruhe Germany

Abstract

Solid‐state‐batteries employing lithium metal anodes promise high theoretical energy and power densities. However, morphological instability occurring at the lithium/solid–electrolyte interface when stripping and plating lithium during cell cycling needs to be mitigated. Vacancy diffusion in lithium metal is not sufficiently fast to prevent pore formation at the interface above a certain current density during stripping. Applied pressure of several MPa can prevent pore formation, but this is not conducive to practical application. This work investigates the concept of ionic liquids as “self‐adjusting” interlayers to compensate morphological changes of the lithium anode while avoiding the use of external pressure. A clear improvement of the lithium dissolution process is observed as it is possible to continuously strip more than 70 μm lithium (i. e., 15 mAh cm ⁻² charge) without the need for external pressure during assembly and electrochemical testing of the system. The impedance of the investigated electrodes is analyzed in detail, and contributions of the different interfaces are evaluated. The conclusions are corroborated with morphology studies using cryo‐FIB‐SEM and chemical analysis using XPS. This improves the understanding of the impedance response and lithium stripping in electrodes employing liquid interlayers, acting as a stepping‐stone for future optimization.

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Sponsoring Organization:: USDOE

OSTI ID:: 1772837

Alternate ID(s):: OSTI ID: 1786226

Journal Information:: Batteries & Supercaps, Journal Name: Batteries & Supercaps Journal Issue: 7 Vol. 4; ISSN 2566-6223

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Working Principle of an Ionic Liquid Interlayer During Pressureless Lithium Stripping on Li _6.25 Al _0.25 La ₃ Zr ₂ O ₁₂ (LLZO) Garnet‐Type Solid Electrolyte