Diluent-mediated interfacial reactions in localized-high-concentration electrolytes for fast-charging lithium-ion batteries

Reframing ionic transport and interface chemistry through electrolyte renovation is essential to promote the fast charging of Li-ion batteries, even under extreme conditions. Despite the formation of a less resistive interface using high-concentration electrolytes (HCEs), their inevitably high visco...

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Published inJournal of materials chemistry. A, Materials for energy and sustainability Vol. 12; no. 27; pp. 16517 - 16527
Main Authors Park, Seungsoo, Chang, Hongjun, Lee, Hyuntae, Lim, Minhong, An, Hyeongguk, Kang, Jiwoong, Lee, Soyeon, Lee, Mingyu, Han, Cheolhee, Lee, Hochun, Chae, Sujong, Moon, Janghyuk, Lee, Hongkyung
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 09.07.2024
Subjects
Charging
Diluents
Electric cells
Electrolytes
Electrolytic cells
Interface reactions
Lithium
Lithium-ion batteries
Low temperature
Rechargeable batteries
Sheaths
Solvation
Viscosity
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Summary:Reframing ionic transport and interface chemistry through electrolyte renovation is essential to promote the fast charging of Li-ion batteries, even under extreme conditions. Despite the formation of a less resistive interface using high-concentration electrolytes (HCEs), their inevitably high viscosity compromises their practical use. This work aims to explore the most suitable hydrofluoroether diluents for localized-high-concentration electrolytes (LHCEs). Contrary to the consensus on their negligible intervention in the Li + solvation sheath, experimental evidence, and simulation studies have revealed that diluents can partially penetrate solvation and enable intermolecular interactions with solvents and additives. While the extent of physical intervention is similar, the intermolecular binding becomes greater when using longer-chain diluents with increased -CF 2 - moieties, hindering the desired interfacial reactions. By strategically selecting smaller diluents with fewer -CF 2 - units, low-viscosity LHCEs can attain the long stable cycling of Li-ion cells at a 10 minute charging rate (∼18 mA cm −2 ) over 500 cycles, and facilitate reliable performance under demanding conditions, such as thick electrodes (∼5 mAh cm −2 ) and low temperatures (−20 °C). The "marionette" effect of various diluents in localized-high-concentration electrolytes subtly controls solvent and additive interactions and refines interfacial chemistry for enhancing Li-ion battery performance, particularly in extreme conditions.
Bibliography:Electronic supplementary information (ESI) available: Supplementary figures. See DOI
Hongkyung Lee is an associate professor in the Department of Energy Science and Engineering at DGIST, South Korea. He earned his PhD in Chemical and Biomolecular Engineering from KAIST in 2016 and conducted postdoctoral research at the Pacific Northwest National Laboratory (PNNL) under the supervision of Dr Ji-Guang Zhang from 2017 to 2019. Throughout his career, Prof. Lee has made significant contributions to the field of advanced battery materials and multi-scale interfacial engineering in Li-metal, Li-sulfur, and Li-air batteries, publishing 86 peer-reviewed articles and securing 19 patents. Currently, his research focuses on dendrite-free electroplating, electrolytes for fast-charging batteries, and imaging-driven battery diagnosis.
https://doi.org/10.1039/d4ta02103g
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ISSN:2050-7488
2050-7496
DOI:10.1039/d4ta02103g