Journal Article

PUBDB-2023-05676

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Electrochemical Stability Window and Electrolyte Breakdown Mechanisms of Lithium Lanthanum Titanate

Ring, J. ; Laa, L. ; Limbeck, A. ; Vonk, V.XFEL.EU*DESY* ; Volkov, S.Extern* ; Nenning, A. (Corresponding author)Extern* ; Fleig, J.Extern*

2023
IOP Publishing Bristol

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Please use a persistent id in citations: doi:10.1149/1945-7111/acd818  doi:10.3204/PUBDB-2023-05676

Abstract: Perovskite-type La$_{0.57}$Li$_{0.29}$TiO$_3$ (LLTO) is a promising solid electrolyte material with high Li-ion conductivity. However, its experimental electrochemical stability window is not precisely known, and thus the compatibility with potential electrode materials is partly unclear. In this contribution, we present results from electrochemical and analytical experiments to elucidate the stability of LLTO when being polarized with Li-ion-blocking Pt electrodes. Above 2.5 V, a darkened color front starts moving from the cathode to the anode, leading to electrolyte degradation. While first-principles calculations predict the appearance of new phases as decomposition products, we find zones with modified defect chemical properties originating from the anode and cathode. The darkened zone forming at the cathode contains Ti$^{3+}$ polarons with high mobility, which leads to a mixed ion-electron conductivity, already for a very small Li excess concentration. Next to the anode a spatially very confined, weakly conductive Li depletion zone forms. The spatially confined but substantial Li depletion near the anode could be quantified by analytical laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). In contrast to first-principles calculations, no new phases were found near the anode, according to synchrotron-based grazing incidence XRD measurements.

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Contributing Institute(s):

1. PETRA-D (FS-PETRA-D)
2. DOOR-User (DOOR ; HAS-User)
3. Nanolab (FS-NL)

Research Program(s):

1. 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) (POF4-632)
2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)

Experiment(s):

1. PETRA Beamline P08 (PETRA III)

Appears in the scientific report 2023

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; IF < 5 ; JCR ; SCOPUS ; Web of Science Core Collection

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