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

机译：用锂金属的石榴石固体电解质界面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：Li7la3zR2O12（LLZO）基于石榴石的材料掺杂有Al，Nb或Ta稳定Li + - 导电立方相是全固态锂金属电池的一种特别有希望的固体电解质。理解固体电解质和相关电极材料之间的内在反应性对于开发具有长寿的高压固态电池至关重要。使用新型的表面科学的方法来表征Li-固体电解质界面的内在反应性，确定令人惊讶的是，所有三种掺杂剂类型都会发生一定程度的Zr还原，随着TA的减少程度增加

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