期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 19, 页码 10871-10879出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202101976
关键词
electrolyte additives; hydrogen bonds; lithium anodes; solid– electrolyte interphase; solvation chemistry
资金
- National Natural Science Foundation of China [51773071, 21873045, 22033004]
- National 1000-Talents Program
- Innovation Fund of WNLO
- Fundamental Research Funds for the Central Universities [HUST: 2018KFYXKJC018, 2019kfyRCPY099]
- State Key Laboratory of Integrated Optoelectronics [IOSKL2020KF02]
- China Postdoctoral Science Foundation [2020M672323]
A novel strategy was proposed to regulate the solvation sheath for improving Li anodes performance, resulting in the formation of robust solid-electrolyte interphase, reduced amount of free solvent molecules, and enhanced stability of electrolytes. This strategy led to improved lithium deposition and impressive electrochemical performance under low coulombic efficiency conditions in experiments.
The performance of Li anodes is extremely affected by the solvation of Li ions, leading to preferential reduction of the solvation sheath and subsequent formation of fragile solid-electrolyte interphase (SEI), Li dendrites, and low coulombic efficiency (CE). Herein, we propose a novel strategy to regulate the solvation sheath, through the introduction of intermolecular hydrogen bonds with both the anions of Li salt and the solvent by small amount additives. The addition of such hydrogen bonds reduced the LUMO energy level of anions in electrolyte, promoted the formation of a robust SEI, reduced the amount of free solvent molecules, and enhanced stability of electrolytes. Based on this strategy, flat and dense lithium deposition was obtained. Even under lean electrolytes, at a current density of 1 mA cm(-2) with a fixed capacity of 3 mAh cm(-2), the Li-Cu cells showed an impressive CE value of 99.2 %. The Li-LiFePO4 full cells showed long-term cycling stability for more than 1000 cycles at 1 C, with a total capacity loss of only 15 mAh g(-1).
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