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Title: Ultrahigh coulombic efficiency electrolyte enables Li||SPAN batteries with superior cycling performance

Journal Article · · Materials Today
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2]
  1. Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering
  2. Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering; Univ. of California, San Diego, CA (United States). Sustainable Power and Energy Center
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Raising the coulombic efficiency of lithium metal anode cycling is the deciding step in realizing long-life rechargeable lithium batteries. Here, we designed a highly concentrated salt/ether electrolyte diluted in a fluorinated ether: 1.8 M LiFSI in DEE/BTFE (diethyl ether/bis(2,2,2-trifluoroethyl)ether), which realized an average coulombic efficiency of 99.37% at 0.5 mA cm-2 and 1 mAh cm-2 for more than 900 cycles. This electrolyte also maintained a record coulombic efficiency of 98.7% at 10 mA cm-2, indicative of its ability to provide fast-charging with high cathode loadings. Morphological studies reveal dense, dendrite free Li depositions after prolonged cycling, while surface analyses confirmed the formation of a robust LiF-rich SEI layer on the cycled Li surface. Moreover, we discovered that this ether-based electrolyte is highly compatible with the low-cost, high-capacity SPAN (Sulfurized polyacrylonitrile) cathode, where the constructed Li||SPAN cell exhibited reversible cathode capacity of 579 mAh g-1 and no capacity decay after 1200 cycles. A cell where a high areal loading SPAN electrode (>3.5 mAh cm-2) is paired with only onefold excess Li was constructed and cycled at 1.75 mA cm-2, maintaining a coulombic efficiency of 99.30% for the lithium metal. Computational simulations revealed that at saturation, the Li-FSI complex forms contact ion pairs, with a first solvation shell comprising DEE molecules, and a second solvation shell with a mix of DEE/BTFE. This study provides a path to enable high energy density Li||SPAN batteries with stable cycling.

Research Organization:
Univ. of California, San Diego, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)
Grant/Contract Number:
EE0007764; CHE‐1338173
OSTI ID:
1848574
Alternate ID(s):
OSTI ID: 1780309
Journal Information:
Materials Today, Vol. 42, Issue C; ISSN 1369-7021
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
77 NANOSCIENCE AND NANOTECHNOLOGY
Materials Science
Ether-based localized high-concentration fluorine-rich electrolytes
Ultrahigh coulombic efficiency
Dendrite free
High energy density
High current density
Li||SPAN battery
Limited Li
Li metal battery
LiF rich SEI