Choi, Jinkwan Jeong, Hyang soo Jang, Juyoung Jeon, A Re Kang, Inyeong Kwon, Minhyung Hong, Ji hyun Lee, Min ah 2024-01-19T14:33:06Z 2024-01-19T14:33:06Z 2021-09-02 2021-06 0002-7863 https://pubs.kist.re.kr/handle/201004/116955 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 highlights the promise of adopting chemical prelithiation for high-capacity anodes to achieve practical high-energy batteries. ？ 2021 American Chemical Society. All rights reserved. English American Chemical Society Weakly Solvating Solution Enables Chemical Prelithiation of Graphite-SiOxAnodes for High-Energy Li-Ion Batteries Article 10.1021/jacs.1c03648 1 Journal of the American Chemical Society, v.143, no.24, pp.9169 - 9176 Journal of the American Chemical Society 143 24 9169 9176 N scie scopus 000667994700026 2-s2.0-85108677118 Chemistry, Multidisciplinary Chemistry Article