Journal
SMALL
Volume 16, Issue 47, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202004688
Keywords
ester electrolytes; high‐ energy‐ density baterries; Li+‐ solvation structure; lithium metal anodes
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Funding
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- University of Waterloo
- Waterloo Institute for Nanotechnology
- Xijiang RD Team
- Special Fund Project of Science and Technology Application in Guangdong [2017B020240002]
- Science and Technology Program of Guangzhou [2019050001]
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The development of high-energy-density Li metal batteries are hindered by electrolyte consumption and uneven lithium deposition due to the unstable lithium-electrolyte interface (SEI). In this work, tetraglyme is introduced into ester electrolyte to regulate the Li+-solvation structures for stable SEI while remaining appropriate voltage window for high-voltage cathodes. In the modified solvation structures, an enhanced lowest unoccupied molecular orbital energy level occurs, resulting in relieved electrolyte degradation. In addition, the modified solvation structures can facilitate adequate LiNO3 dissolution in the ester electrolyte (denoted as E-LiNO3), contributing to constant supplement of constructing highly conductive LiNxOy-containing SEI for dendrite-free Li deposition under high capacity condition. As a result, the Li||Cu cell-based on this electrolyte exhibits high Li plating/stripping Coulombic efficiency of 98.2% over 350 cycles. Furthermore, when paired with high-voltage LiNi0.5Co0.2Mn0.3O2 cathodes, the E-LiNO3 enables a stable cycling with a high-energy-density of 296 Wh kg(-1) based on the full cell under realistic testing conditions (lean electrolyte of 3 g Ah(-1), limited Li excess of 2.45-fold, and high areal capacity of 4 mAh cm(-2)).
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