Weakly Solvating Solution Enables Chemical Prelithiation of Graphite-SiOx Anodes for High-Energy Li-Ion Batteries.

Journal of the American Chemical Society
Jinkwan ChoiMinah Lee

Abstract

Although often overlooked in anode research, the anode's initial Coulombic efficiency (ICE) is a crucial factor dictating the energy density of a practical Li-ion battery. For next-generation anodes, a blend of graphite and Si/SiOx represents the most practical way to balance capacity and cycle life, but its low ICE limits its commercial viability. Here, we develop a chemical prelithiation method to maximize the ICE of the blend anodes using a reductive Li-arene complex solution of regulated solvation power, which enables a full cell to exhibit a near-ideal energy density. To prevent structural degradation of the blend during prelithiation, we investigate a solvation rule to direct the Li+ intercalation mechanism. Combined spectroscopy and density functional theory calculations reveal that in weakly solvating solutions, where the Li+-anion interaction is enhanced, free solvated-ion formation is inhibited during Li+ desolvation, thereby mitigating solvated-ion intercalation into graphite and allowing stable prelithiation of the blend. Given the ideal ICE of the prelithiated blend anode, a full cell exhibits an energy density of 506 Wh kg-1 (98.6% of the ideal value), with a capacity retention after 250 cycles of 87.3%. This work...Continue Reading

References

Nov 17, 2001·Chemical Reviews·K B Wiberg
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Jan 31, 2018·Accounts of Chemical Research·Lidan XingWeishan Li
Nov 21, 2018·Chemical Society Reviews·Zhenhui LiuLiqiang Mai
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Aug 9, 2019·ACS Applied Materials & Interfaces·Qinghai MengYu-Guo Guo
Dec 15, 2020·ACS Applied Materials & Interfaces·Wenquan LuLikun Zhu

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Citations

Nov 23, 2021·Advanced Materials·Yanqun LvShimou Chen

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