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Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries

Journal Article · · Nature Energy
 [1];  [1];  [1];  [2];  [2];  [3];  [4];  [1];  [1];  [1];  [2];  [3];  [2];  [4];  [5];  [1]
  1. Univ. of Maryland, College Park, MD (United States)
  2. Rutgers Univ., New Brunswick, NJ (United States); The State Univ. of New Jersey, New Brunswick, NJ (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. US Army Combat Capabilities Development Command Army Research Laboratory, Adelphi, MA (United States)
+ Show Author Affiliations
Lithium batteries with Si, Al or Bi microsized (>10 µm) particle anodes promise a high capacity, ease of production, low cost and low environmental impact, yet they suffer from fast degradation and a low Coulombic efficiency. In this paper, we demonstrate that a rationally designed electrolyte (2.0 M LiPF6 in 1:1 v/v mixture of tetrahydrofuran and 2-methyltetrahydrofuran) enables 100 cycles of full cells that contain microsized Si, Al and Bi anodes with commercial LiFePO4 and LiNi0.8Co0.15Al0.05O2 cathodes. Alloy anodes with areal capacities of more than 2.5 mAh cm-2 achieved >300 cycles with a high initial Coulombic efficiency of >90% and average Coulombic efficiency of >99.9%. These improvements are facilitated by the formation of a high-modulus LiF–organic bilayer interphase, in which LiF possesses a high interfacial energy with the alloy anode to accommodate plastic deformation of the lithiated alloy during cycling. Lastly, this work provides a simple yet practical solution to current battery technology without any binder modification or special fabrication methods.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC05-76RL01830; EE0008202; SC0012704
OSTI ID:
1619250
Alternate ID(s):
OSTI ID: 1633614
Report Number(s):
BNL--215931-2020-JAAM; PNNL-SA--151702
Journal Information:
Nature Energy, Journal Name: Nature Energy Journal Issue: 5 Vol. 5; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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