Building Lithiophilic Ion‐Conduction Highways on Garnet‐Type Solid‐State Li+ Conductors,Advanced Energy Materials

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Building Lithiophilic Ion‐Conduction Highways on Garnet‐Type Solid‐State Li+ Conductors
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-05-07 , DOI: 10.1002/aenm.201904230
Zhangyuan Cheng ₁ , Maoling Xie ₁ , Yayun Mao ₂ , Jianxin Ou ₁ , Sijing Zhang ₁ , Zheng Zhao ₁ , Jinlin Li ₁ , Fang Fu ₁ , Jihuai Wu ₁ , Yanbin Shen ₂ , Derong Lu ₃ , Hongwei Chen ₁

Affiliation

The integration of highly conductive solid‐state electrolytes (SSEs) into solid‐state cells is still a challenge mainly due to the high impedance existing at the electrolyte/electrode interface. Although solid‐state garnet‐based batteries have been successfully assembled with the assistance of an intermediate layer between the garnet and the Li metal anode, the slow discharging/charging rates of the batteries inhibits practical applications, which require much higher power densities. Here, a crystalline sulfonated‐covalent organic framework (COF) thin layer is grown on the garnet surface via a simple solution process. It not only significantly improves the lithiophilicity of garnet electrolytes via the lithiation of the COF layer with molten Li, but also creates effective Li⁺ diffusion “highways” between the garnet and the Li metal anode. As a result, the interfacial impedance of symmetric solid‐state Li cells is significantly decreased and the cells can be operated at high current densities up to 3 mA cm⁻², which is difficult to achieve with current interfacial modification technologies for SSEs. The solid‐state Li‐ion batteries using LiFePO₄ cathodes, Li anodes, and COF‐modified garnet electrolytes thus exhibit a significantly improved rate capability.

中文翻译：

在石榴石型固态Li +导体上建造亲硫离子传导高速公路

将高导电性固态电解质（SSE）集成到固态电池中仍然是一个挑战，主要是因为电解质/电极界面处存在高阻抗。尽管已经在石榴石和锂金属阳极之间的中间层的帮助下成功地组装了基于石榴石的固态电池，但是电池的缓慢放电/充电速率阻碍了实际应用，因为实际应用需要更高的功率密度。在这里，通过简单的溶解过程，在石榴石表面上生长了结晶的磺化共价有机骨架（COF）薄层。它不仅可以通过COF层与熔融Li的锂化来显着提高石榴石电解质的耐锂亲和性，还可以产生有效的Li ⁺石榴石和锂金属阳极之间的“高速”扩散。结果，对称固态锂电池的界面阻抗显着降低，并且这些电池可以在高达3 mA cm ^-2的高电流密度下运行，这很难通过当前的SSE界面改性技术来实现。因此，使用LiFePO ₄阴极，Li阳极和COF改性石榴石电解质的固态锂离子电池具有显着提高的倍率能力。

更新日期：2020-06-23

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