A High-Performance Carbonate-Free Lithium|Garnet Interface Enabled by a Trace Amount of Sodium.,Advanced Materials

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A High-Performance Carbonate-Free Lithium|Garnet Interface Enabled by a Trace Amount of Sodium.
Advanced Materials ( IF 27.4 ) Pub Date : 2020-05-25 , DOI: 10.1002/adma.202000575
Xingjie Fu ₁ , Tiantian Wang ₂ , Wenzhong Shen ₁ , Miaoli Jiang ₁ , Youwei Wang ₂ , Qiushi Dai ₃ , Da Wang ₁ , Zhenping Qiu ₁ , Yelong Zhang ₁ , Kuirong Deng ₁ , Qingguang Zeng ₁ , Ning Zhao ₄ , Xiangxin Guo ₄ , Zheng Liu _{1,

5} , Jianjun Liu ₂ , Zhangquan Peng _{1,

6}

Affiliation

Garnet‐type solid‐state electrolytes (SSEs) are promising for the realization of next‐generation high‐energy‐density Li metal batteries. However, a critical issue associated with the garnet electrolytes is the poor physical contact between the Li anode and the garnet SSE and the resultant high interfacial resistance. Here, it is reported that the Li|garnet interface challenge can be addressed by using Li metal doped with 0.5 wt% Na (denoted as Li*) and melt‐casting the Li* onto the garnet SSE surface. A mechanistic study, using Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) as a model SSE, reveals that Li₂CO₃ resides within the grain boundaries of newly polished LLZTO pellet, which is difficult to remove and hinders the wetting process. The Li* melt can phase‐transfer the Li₂CO₃ from the LLZTO grain boundary to the Li*’s top surface, and therefore facilitates the wetting process. The obtained Li*|LLZTO demonstrates a low interfacial resistance, high rate capability, and long cycle life, and can find applications in future all‐solid‐state batteries (e.g., Li*|LLZTO|LiFePO₄).

中文翻译：

微量的钠实现了高性能的无碳酸盐锂/石榴石界面。

石榴石型固态电解质（SSE）对于实现下一代高能量密度锂金属电池很有希望。然而，与石榴石电解质有关的一个关键问题是锂阳极与石榴石SSE之间的不良物理接触以及由此产生的高界面电阻。在这里，据报道，可以通过使用掺杂有0.5 wt％Na（表示为Li *）的Li金属并将Li *熔铸到石榴石SSE表面上来解决锂石榴石界面难题。使用Li _6.4 La ₃ Zr _1.4 Ta _0.6 O ₁₂（LLZTO）作为模型SSE的机理研究表明Li ₂ CO ₃残留在新抛光的LLZTO颗粒的晶界内，这很难去除并阻碍了润湿过程。Li *熔体可以将Li ₂ CO ₃从LLZTO晶界相转移到Li *的上表面，因此有利于润湿过程。所获得的Li * | LLZTO具有低的界面电阻，高倍率能力和长循环寿命，并且可以在未来的全固态电池（例如Li * | LLZTO | LiFePO ₄）中找到应用。

更新日期：2020-07-01

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