Anion-Reinforced Solvating Ionic Liquid Electrolytes Enabling Stable High-Nickel Cathode in Lithium-Metal Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 38336365.
- Also identified by DOI 10.1002/adma.202400537.
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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<sup>+</sup> 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<sup>+</sup> to address this concern. The designed ASILEs, incorporating chlorinated hydrocarbons and two anions, bis(fluorosulfonyl) imide (FSI<sup>-</sup>) and bis(trifluoromethanesulfonyl) imide (TFSI<sup>-</sup>), aim to enhance Li<sup>+</sup> transport ability, stabilize the interface of the high-nickel cathode material (LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>, NCM811), and retain fire-retardant properties. With these ASILEs, the Li/NCM811 cell exhibits high initial specific capacity (203 mAh g<sup>-1</sup> 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<sup>-1</sup>, 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.