Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 24, Pages 9169-9176Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c03648
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Funding
- Korea Institute of Science and Technology (KIST) [2E30993, 2E30991, 2V09112]
- National Research Foundation of Korea (NRF) - Korea government (MSIT) [2020M1A2A2080881, 2020M3H4A1A03082978, 2021R1A2C2006243, 2021R1C1C1006721]
- National Research Foundation of Korea [2021R1A2C2006243, 2020M1A2A2080881, 2020M3H4A1A03082978, 2021R1C1C1006721] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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The initial Coulombic efficiency of the anode is crucial for the energy density of a Li-ion battery, and a blend of graphite and Si/SiOx is the most practical way to balance capacity and cycle life, but its low ICE limits its commercial viability. A chemical prelithiation method can maximize the ICE of the blend anodes, leading to a near-ideal energy density in a full cell.
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.
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