Abstract:
Ionic liquid electrolytes (ILEs) are promising to develop high‐safety and high‐energy‐density lithium‐metal batteries (LMBs). Unfortunately, ILEs normally face the challenge of sluggish Li+ transport due to increased ions’ clustering caused by Coulombic interactions. Here a type of anion‐reinforced solvating ILEs (ASILEs) is discovered, which reduce ions’ clustering by enhancing the anion–cation coordination and promoting more anions to enter the internal solvation sheath of Li+ to address this concern. The designed ASILEs, incorporating chlorinated hydrocarbons and two anions, bis(fluorosulfonyl) imide (FSI−) and bis(trifluoromethanesulfonyl) imide (TFSI−), aim to enhance Li+ transport ability, stabilize the interface of the high‐nickel cathode material (LiNi0.8Co0.1Mn0.1O2, NCM811), and retain fire‐retardant properties. With these ASILEs, the Li/NCM811 cell exhibits high initial specific capacity (203 mAh g−1 at 0.1 C), outstanding capacity retention (81.6% over 500 cycles at 1.0 C), and excellent average Coulombic efficiency (99.9% over 500 cycles at 1.0 C). Furthermore, an Ah‐level Li/NCM811 pouch cell achieves a notable energy density of 386 Wh kg−1, indicating the practical feasibility of this electrolyte. This research offers a practical solution and fundamental guidance for the rational design of advanced ILEs, enabling the development of high‐safety and high‐energy‐density LMBs.
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Advanced Materials
ISSN: 0935-9648
Year: 2024
Issue: 23
Volume: 36
Page: n/a-n/a
2 7 . 4 0 0
JCR@2023
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30 Days PV: 1
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