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Dopant-Dependent Stability of Garnet Solid Electrolyte Interfaces with Lithium Metal

机译：石榴石固体电解质与锂金属的掺杂剂依赖性稳定性

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摘要

Li7La3Zr2O12(LLZO) garnet-based materials doped with Al, Nb, or Ta to stabilize the Li+-conductive cubic phase are a particularly promising class of solid electrolytes for all-solid-state lithium metal batteries. Understanding of the intrinsic reactivity between solid electrolytes and relevant electrode materials is crucial to developing high voltage solid-state batteries with long lifetimes. Using a novel, surface science-based approach to characterize the intrinsic reactivity of the Li-solid electrolyte interface, it is determined that, surprisingly, some degree of Zr reduction takes place for all three dopant types, with the extent of reduction increasing as Ta Nb Al. Significant reduction of Nb also takes place for Nb-doped LLZO, with electrochemical impedance spectroscopy (EIS) of Li parallel to Nb-LLZO parallel to Li symmetric cells further revealing significant increases in impedance with time and suggesting that the Nb reduction propagates into the bulk. Density functional theory (DFT) calculations reveal that Nb-doped material shows a strong preference for Nb dopants toward the interface between LLZO and Li, while Ta does not exhibit a similar preference. EIS and DFT results, coupled with the observed reduction of Zr at the interface, are consistent with the formation of an "oxygen-deficient interphase" (ODI) layer whose structure determines the stability of the LLZO-Li interface.
机译：掺杂Al，Nb或Ta来稳定Li +导电立方相的Li7La3Zr2O12（LLZO）石榴石基材料是用于全固态锂金属电池的一类特别有前景的固体电解质。了解固体电解质和相关电极材料之间的固有反应性对于开发使用寿命长的高压固态电池至关重要。使用一种新颖的，基于表面科学的方法来表征锂固体电解质界面的固有反应性，可以确定的是，令人惊奇的是，所有三种掺杂剂都发生了一定程度的Zr还原，还原程度随着Ta的增加而增加

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