Defect chemistry engineering of Ga-doped garnet electrolyte with high stability for solid-state lithium metal batteries

IF 16.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Accounts of Chemical Research Pub Date : 2024-04-23 DOI:10.1088/1674-1056/ad41b9

Sihan Chen, Jun Li, Keke Liu, Xiaochen Sun, Jingwei Wan, Huiyu Zhai, Xinfeng Tang, G. Tan

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Abstract

Ga-doped Li7La3Zr2O12 (Ga-LLZO) has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries (ASSLBs) due to its high room temperature ionic conductivity. However, the typical synthesis of Ga-LLZO is usually accompanied by the formation of undesired LiGaO2 impurity phase that causes severe instability issue of electrolyte in contact with molten Li metal during half/full cells assembly. In this study, we show that by simply engineering the defect chemistry of Ga-LLZO, namely, the lithium deficiency level, LiGaO2 impurity phase is effectively inhibited in the final synthetic product. Consequently, defect chemistry engineered Ga-LLZO exhibits excellent electrochemical stability against lithium metal, while its high room temperature ionic conductivity (~1.9 × 10-3 S·cm-1) is well reserved. The assembled Li/Ga-LLZO/Li symmetric cell has a superior critical current density of 0.9 mA·cm-2, and cycles stably for 500 hours at a current density of 0.3 mA·cm-2. This research facilitates the potential commercial applications of high performance Ga-LLZO solid electrolyte in ASSLBs.

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用于固态锂金属电池的高稳定性掺镓石榴石电解质的缺陷化学工程

掺杂镓的 Li7La3Zr2O12（Ga-LLZO）因其室温离子电导率高，长期以来一直被认为是全固态锂金属电池（ASSLB）的理想石榴石型电解质。然而，Ga-LLZO 的典型合成通常会伴随着不受欢迎的 LiGaO2 杂质相的形成，从而导致电解质在半/全电池组装过程中与熔融锂金属接触时出现严重的不稳定问题。在本研究中，我们发现只需对 Ga-LLZO 的缺陷化学（即锂缺乏水平）进行设计，就能有效抑制最终合成产品中的 LiGaO2 杂质相。因此，缺陷化学工程 Ga-LLZO 对锂金属具有优异的电化学稳定性，同时还保留了较高的室温离子电导率（约 1.9 × 10-3 S-cm-1）。组装好的锂/镓-LLZO/锂对称电池的临界电流密度高达 0.9 mA-cm-2，并能在 0.3 mA-cm-2 的电流密度下稳定循环 500 小时。这项研究促进了高性能 Ga-LLZO 固体电解质在 ASSLB 中的潜在商业应用。

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来源期刊

Accounts of Chemical Research 化学-化学综合

CiteScore

31.40

自引率

1.10%

发文量

312

审稿时长

2 months

期刊介绍： Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.