Issue 9, 2023

Benchmarking the performance of lithiated metal oxide interlayers at the LiCoO2|LLZO interface

Abstract

Integrating Li7La3Zr2O12 (LLZO) solid-state electrolytes in combination with a high-energy cathode remains a major challenge in developing all-solid-state batteries. In particular, diffusion processes and solid-state reactions at the cathode–electrolyte interface during the co-sintering of the oxide materials at elevated temperatures result in high interfacial impedances. In this work, we study the performance of lithiated Nb, Al, and Ti metal oxide interlayers as diffusion barriers to prevent the formation of deleterious interphases at the cathode–electrolyte interface during fabrication, thus enabling easy Li-ion transfer between LiCoO2 and LLZO. Specifically, we characterize the impact of the different interlayers on the morphology and elemental distribution at the interface and evaluate their influence on the electrochemical behavior of the battery stacks after the high-temperature process. We find that the mixing of Co/La cations at the interface is reduced by using the metal oxide diffusion barriers. It is shown that the interfacial impedance can be reduced from 8 kΩ cm2 to 1 kΩ cm2 and that the electrochemical performance of all cells with interlayers exceeds that of the battery without interlayer. In particular, the Li–Nb–O modification outperforms the other metal oxide interlayers in terms of the discharge capacities achieved.

Graphical abstract: Benchmarking the performance of lithiated metal oxide interlayers at the LiCoO2|LLZO interface

Supplementary files

Article information

Article type
Paper
Submitted
02 apr 2023
Accepted
04 apr 2023
First published
17 apr 2023
This article is Open Access
Creative Commons BY-NC license

Mater. Adv., 2023,4, 2138-2146

Benchmarking the performance of lithiated metal oxide interlayers at the LiCoO2|LLZO interface

A. Müller, F. Okur, A. Aribia, N. Osenciat, C. A. F. Vaz, V. Siller, M. El Kazzi, E. Gilshtein, M. H. Futscher, K. V. Kravchyk, M. V. Kovalenko and Y. E. Romanyuk, Mater. Adv., 2023, 4, 2138 DOI: 10.1039/D3MA00155E

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