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Title: Anion-tethered Single Lithium-ion Conducting Polyelectrolytes through UV-induced Free Radical Polymerization for Improved Morphological Stability of Lithium Metal Anodes

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of California, Irvine, CA (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
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Single Li+ ion conducting polyelectrolytes (SICs), which feature covalently tethered counter-anions along their backbone, have the potential to mitigate dendrite formation by reducing concentration polarization and preventing salt depletion. However, due to their low ionic conductivity and complicated synthetic procedure, the successful validation of these claimed advantages in lithium metal (Li0) anode batteries remains limited. In this study, we fabricated a SIC electrolyte using a single-step UV polymerization approach. The resulting electrolyte exhibited a high Li+ transference number (t+) of 0.85 and demonstrated good Li+ conductivity (6.3×10-5 S/cm at room temperature), which is comparable to that of a benchmark dual ion conductor (DIC, 9.1×10-5 S/cm). Benefitting from the high transference number of SIC, it displayed a three-fold higher critical current density (2.4 mA/cm2) compared to DIC (0.8 mA/cm2) by successfully suppressing concentration polarization-induced short-circuiting. Additionally, the t+ significantly influenced the deposition behavior of Li0, with SIC yielding a uniform, compact, and mosaic-like morphology, while the low t+ DIC resulted in a porous morphology with Li0 whiskers. In conclusion, using the SIC electrolyte, Li0||LiFePO4 cells exhibited stable operation for 4500 cycles with 70.5 % capacity retention at 22 °C.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704; SC0021204
OSTI ID:
2008214
Report Number(s):
BNL--224884-2023-JAAM
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 38 Vol. 62; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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25 ENERGY STORAGE
lithium metal battery
polyelectrolyte
polymer electrolytes
single Li+ conductor
solid state batteries
transference number