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Title: High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode

Journal Article · · Advanced Functional Materials
ORCiD logo [1]; ORCiD logo [2];  [3];  [2];  [4]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [4];  [5]; ORCiD logo [2];  [6]; ORCiD logo [1]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  3. Univ. of California San Diego, La Jolla, CA (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  6. Univ. of California San Diego, La Jolla, CA (United States); Univ. of Chicago, IL (United States)

The practical application of lithium (Li) metal anode (LMA) is still hindered by non-uniformity of solid electrolyte interphase (SEI), formation of "dead" Li, and continuous consumption of electrolyte although LMA has an ultrahigh theoretical specific capacity and a very low electrochemical redox potential. Herein, we report a facile protection strategy for LMA using a double layer (DL) coating that consists of a polyethylene oxide (PEO)-based bottom layer which is highly stable with LMA and promotes uniform ion flux, and a cross-linked polymer-based top layer which prevents solvation of PEO layer in electrolytes. Li deposited on DL-coated Li (DL@Li) exhibits a smoother surface and much larger size than that deposited on bare Li. The LiF/Li2O enriched SEI layer generated by the salt decomposition on top of DL@Li further suppresses the side reactions between Li and electrolyte. Driven by the abovementioned advantageous features, the DL@Li||LiNi0.6Mn0.2Co0.2O2 cells demonstrate capacity retention of 92.4% after 220 cycles at a current density of 2.1 mA cm-2 (C/2 rate) and stability at a high charging current density of 6.9 mA cm-2 (1.5C rate). These results indicate that the DL protection is promising to overcome the rate limitation of LMAs and high energy-density Li metal batteries.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Science Foundation (NSF); USDOE Office of Science (SC)
Grant/Contract Number:
SC0012704; AC05-76RL01830; ECCS-1542148
OSTI ID:
1891326
Report Number(s):
BNL-223535-2022-JAAM
Journal Information:
Advanced Functional Materials, Vol. 32, Issue 48; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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