Improving cyclability of Li metal batteries at elevated temperatures and its origin revealed by cryo-electron microscopy

Jiangyan Wang, William Huang, Allen Pei, Yuzhang Li, Feifei Shi, Xiaoyun Yu and Yi Cui ()
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Jiangyan Wang: Stanford University
William Huang: Stanford University
Allen Pei: Stanford University
Yuzhang Li: Stanford University
Feifei Shi: Stanford University
Xiaoyun Yu: Stanford University
Yi Cui: Stanford University

Nature Energy, 2019, vol. 4, issue 8, 664-670

Abstract: Abstract Operations of lithium-ion batteries have long been limited to a narrow temperature range close to room temperature. At elevated temperatures, cycling degradation speeds up due to enhanced side reactions, especially when high-reactivity lithium metal is used as the anode. Here, we demonstrate enhanced performance in lithium metal batteries operated at elevated temperatures. In an ether-based electrolyte at 60 °C, an average Coulombic efficiency of 99.3% is obtained and more than 300 stable cycles are realized, but, at 20 °C, the Coulombic efficiency drops dramatically within 75 cycles, corresponding to an average Coulombic efficiency of 90.2%. Cryo-electron microscopy reveals a drastically different solid electrolyte interface nanostructure emerging at 60 °C, which maintains mechanical stability, inhibits continuous side reactions and guarantees good cycling stability and low electrochemical impedance. Furthermore, larger lithium particles grown at the elevated temperature reduce the electrolyte/electrode interfacial area, which decreases the per-cycle lithium loss and enables higher Coulombic efficiencies.

Date: 2019
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DOI: 10.1038/s41560-019-0413-3

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