Dual-Solvent Li-Ion Solvation Enables High-Performance Li-Metal Batteries

Wang, Hansen; Yu, Zhiao; Kong, Xian; Huang, William; Zhang, Zewen; Mackanic, David G.; Huang, Xinyi; Qin, Jian; Bao, Zhenan; Cui, Yi

doi:10.1002/adma.202008619

Dual-Solvent Li-Ion Solvation Enables High-Performance Li-Metal Batteries

Journal Article · Sun May 09 00:00:00 EDT 2021 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202008619· OSTI ID:1787601

^[1]; Yu, Zhiao ^[1]; Kong, Xian ^[1]; Huang, William ^[1]; Zhang, Zewen ^[1]; Mackanic, David G. ^[1]; Huang, Xinyi ^[1]; Qin, Jian ^[1]; Bao, Zhenan ^[1]; Cui, Yi ^[2]

Stanford Univ., CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

Novel electrolyte designs to further enhance the lithium (Li) metal battery cyclability are highly desirable. Here, fluorinated 1,6-dimethoxyhexane (FDMH) is designed and synthesized as the solvent molecule to promote electrolyte stability with its prolonged –CF₂– backbone. Meanwhile, 1,2-dimethoxyethane is used as a co-solvent to enable higher ionic conductivity and much reduced interfacial resistance. Combining the dual-solvent system with 1 m lithium bis(fluorosulfonyl)imide (LiFSI), high Li-metal Coulombic efficiency (99.5%) and oxidative stability (6 V) are achieved. Using this electrolyte, 20 µm Li||NMC batteries are able to retain ≈80% capacity after 250 cycles and Cu||NMC anode-free pouch cells last 120 cycles with 75% capacity retention under ≈2.1 µL mAh^-1 lean electrolyte conditions. Such high performances are attributed to the anion-derived solid-electrolyte interphase, originating from the coordination of Li-ions to the highly stable FDMH and multiple anions in their solvation environments. This work demonstrates a new electrolyte design strategy that enables high-performance Li-metal batteries with multisolvent Li-ion solvation with rationally optimized molecular structure and ratio.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1787601

Alternate ID(s):: OSTI ID: 1782365

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 25 Vol. 33; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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