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

Abstract

Abstract 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 –CF 2 – 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  µ m 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  µ L 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.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Science Foundation (NSF)
OSTI Identifier:
1787601
Alternate Identifier(s):
OSTI ID: 1782365
Grant/Contract Number:  
AC02-76SF00515; ECCS‐1542152
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 33; Journal Issue: 25; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; anode-free batteries; Coulombic efficiency; electrolytes; fluorinated solvents; Li-metal batteries

Citation Formats

Wang, Hansen, Yu, Zhiao, Kong, Xian, Huang, William, Zhang, Zewen, Mackanic, David G., Huang, Xinyi, Qin, Jian, Bao, Zhenan, and Cui, Yi. Dual-Solvent Li-Ion Solvation Enables High-Performance Li-Metal Batteries. United States: N. p., 2021. Web. doi:10.1002/adma.202008619.
Wang, Hansen, Yu, Zhiao, Kong, Xian, Huang, William, Zhang, Zewen, Mackanic, David G., Huang, Xinyi, Qin, Jian, Bao, Zhenan, & Cui, Yi. Dual-Solvent Li-Ion Solvation Enables High-Performance Li-Metal Batteries. United States. https://doi.org/10.1002/adma.202008619
Wang, Hansen, Yu, Zhiao, Kong, Xian, Huang, William, Zhang, Zewen, Mackanic, David G., Huang, Xinyi, Qin, Jian, Bao, Zhenan, and Cui, Yi. Sun . "Dual-Solvent Li-Ion Solvation Enables High-Performance Li-Metal Batteries". United States. https://doi.org/10.1002/adma.202008619. https://www.osti.gov/servlets/purl/1787601.
@article{osti_1787601,
title = {Dual-Solvent Li-Ion Solvation Enables High-Performance Li-Metal Batteries},
author = {Wang, Hansen and Yu, Zhiao and Kong, Xian and Huang, William and Zhang, Zewen and Mackanic, David G. and Huang, Xinyi and Qin, Jian and Bao, Zhenan and Cui, Yi},
abstractNote = {Abstract 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 –CF 2 – 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  µ m 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  µ L 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.},
doi = {10.1002/adma.202008619},
journal = {Advanced Materials},
number = 25,
volume = 33,
place = {United States},
year = {Sun May 09 00:00:00 EDT 2021},
month = {Sun May 09 00:00:00 EDT 2021}
}

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