Engineering a passivating electric double layer for high performance lithium metal batteries

Weili Zhang, Yang Lu, Lei Wan, Pan Zhou, Yingchun Xia, Shuaishuai Yan, Xiaoxia Chen, Hangyu Zhou, Hao Dong and Kai Liu ()
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Weili Zhang: Tsinghua University
Yang Lu: Tsinghua University
Lei Wan: Tsinghua University
Pan Zhou: Tsinghua University
Yingchun Xia: Tsinghua University
Shuaishuai Yan: Tsinghua University
Xiaoxia Chen: Tsinghua University
Hangyu Zhou: Tsinghua University
Hao Dong: Tsinghua University
Kai Liu: Tsinghua University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract In electrochemical devices, such as batteries, traditional electric double layer (EDL) theory holds that cations in the cathode/electrolyte interface will be repelled during charging, leaving a large amount of free solvents. This promotes the continuous anodic decomposition of the electrolyte, leading to a limited operation voltage and cycle life of the devices. In this work, we design a new EDL structure with adaptive and passivating properties. It is enabled by adding functional anionic additives in the electrolyte, which can selectively bind with cations and free solvents, forming unique cation-rich and branch-chain like supramolecular polymer structures with high electrochemical stability in the EDL inner layer. Due to this design, the anodic decomposition of ether-based electrolytes is significantly suppressed in the high voltage cathodes and the battery shows outstanding performances such as super-fast charging/discharging and ultra-low temperature applications, which is extremely hard in conventional electrolyte design principle. This unconventional EDL structure breaks the inherent perception of the classical EDL rearrangement mechanism and greatly improve electrochemical performances of the device.

Date: 2022
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DOI: 10.1038/s41467-022-29761-z

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