Nano Energy, volume 92, pages 106758
Structural origin of low Li-ion conductivity in perovskite solid-state electrolyte
Publication type: Journal Article
Publication date: 2022-02-01
General Materials Science
Electrical and Electronic Engineering
Renewable Energy, Sustainability and the Environment
Abstract
Perovskite solid-state electrolyte, Lithium Lanthanum Titanium Oxide, has long been considered as a promising candidate enabling all-solid-state Li batteries due to its high bulk Li-ion conductivity and wide electrochemical window. However, the Li-ion conductivity at so called “grain boundaries” (GBs) off LLTO pellets is much lower than that of its bulk phase. Thus, understanding the structural origin of the low Li-ion conductivity of LLTO is critical yet remains largely elusive. Here, we identify two types of GBs at different length scales, namely “macro” and “micro” GBs in LLTO pellets and originate them to the processing of LLTO. We also find a nanosized Li-poor orthogonal phase at micro-GBs, which largely deteriorate the Li conduction. Corroborated by electrochemical measurements, we revealed the phase transformation from tetragonal Li 0.33 La 0.56 TiO 3 to orthogonal Li 0.18 La 0.6 TiO 3 during the heat-treatment process is responsible for this deterioration. During phase transformation process, La atoms move to the original Li-rich layer and block the diffusion path of Li-ions in LLTO. These results reveal the structural origin of low Li-ion conductivity in LLTO pellets and provide insights to prevent Li-loss induced phase transformation for commercial application of LLTO. • Two types of grains and corresponding boundaries are identified in LLTO pellets at different length scales, macro vs. micro. • A Li-poor phase has been found existed at both grain boundaries. • The tetra-LLTO phase transition to the Li-poor ortho-phase is due to the heat-treatment when preparing the LLTO pellets. • The existence of hierarchical grain boundaries and Li-poor phase collectively affect the Li-ion conduction in LLTO pellets.
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Xu L. et al. Structural origin of low Li-ion conductivity in perovskite solid-state electrolyte // Nano Energy. 2022. Vol. 92. p. 106758.
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Xu L., Zhang L., Hu Y., Luo L. Structural origin of low Li-ion conductivity in perovskite solid-state electrolyte // Nano Energy. 2022. Vol. 92. p. 106758.
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TY - JOUR
DO - 10.1016/j.nanoen.2021.106758
UR - https://doi.org/10.1016/j.nanoen.2021.106758
TI - Structural origin of low Li-ion conductivity in perovskite solid-state electrolyte
T2 - Nano Energy
AU - Xu, Lei
AU - Zhang, Lifeng
AU - Hu, Yubing
AU - Luo, Langli
PY - 2022
DA - 2022/02/01 00:00:00
PB - Elsevier
SP - 106758
VL - 92
SN - 2211-2855
ER -
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@article{2022_Xu,
author = {Lei Xu and Lifeng Zhang and Yubing Hu and Langli Luo},
title = {Structural origin of low Li-ion conductivity in perovskite solid-state electrolyte},
journal = {Nano Energy},
year = {2022},
volume = {92},
publisher = {Elsevier},
month = {feb},
url = {https://doi.org/10.1016/j.nanoen.2021.106758},
pages = {106758},
doi = {10.1016/j.nanoen.2021.106758}
}
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