Electrolyte solvation chemistry to construct an anion-tuned interphase for stable high-temperature lithium metal batteries

Lithium metal batteries are regarded as promising alternative next-generation energy storage systems. However, the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency (CE). Herein, we rationally design a Li+ coordination structure v...

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Bibliographic Details
Main Authors: Jiahang Chen, Yang Zhang, Huichao Lu, Juan Ding, Xingchao Wang, Yudai Huang, Huiyang Ma, Jiulin Wang
Format: Article
Language:English
Published: KeAi Communications Co. Ltd. 2023-08-01
Series:eScience
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Online Access:http://www.sciencedirect.com/science/article/pii/S2667141723000605
Description
Summary:Lithium metal batteries are regarded as promising alternative next-generation energy storage systems. However, the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency (CE). Herein, we rationally design a Li+ coordination structure via electrolyte solvation chemistry. Nitrate anions are aggregated in the solvation sheath, even at low concentration in a solvent with moderate solvation ability, which promotes Li+ desolvation and constructs a nitrate anion-tuned interphase. Meanwhile, a high-donor-number solvent is introduced as an additive to strongly coordinate with Li+, which accelerates the ion-transfer kinetics and rate performance. This not only results in micro-sized lithium deposition and a high CE of 99.5% over 3500 ​h, but also enables superior anode stability even under 50% depth plating/stripping and with a lean electrolyte of 3 ​g ​Ah−1 at 50 ​°C. A lithium–sulfur battery exhibits a prolonged lifespan of 2000 cycles with an average CE of 100%. A full battery using 1x excess lithium exhibits a high capacity near 1600 ​mAh ​gS−1 for 100 cycles without capacity loss. Moreover, a 0.55 ​Ah pouch cell delivers a reversible energy density of 423 ​Wh ​kg−1 based on these electrodes and electrolyte.
ISSN:2667-1417