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Title: Effects of Imide-Orthoborate Dual-Salt Mixtures in Organic Carbonate Electrolytes on the Stability of Lithium Metal Batteries

The effects of lithium imide and lithium orthoborate dual-salt electrolytes of different salt chemistries in carbonate solvents on the cycling stability of lithium (Li) metal batteries are systematically and comparatively investigated. Two imide salts (LiTFSI and LiFSI) and two orthoborate salts (LiBOB and LiDFOB) are chosen for this study and compared with the conventional LiPF6 salt. Density functional theory calculations indicate that the chemical and electrochemical stabilities follow the order of LiTFSI-LiBOB > LiTFSI-LiDFOB > LiFSI-LiDFOB > LiFSI-LiBOB. The experimental cycling stability of the Li metal batteries with the electrolytes follows the order as LiTFSI-LiBOB > LiTFSI-LiDFOB > LiFSI-LiDFOB > LiPF6 > LiFSI-LiBOB, which is in well accordance with the calculation results. The LiTFSI-LiBOB can effectively protect the Al substrate and form a more robust surface film on Li metal anode, while the LiFSI-LiBOB results in serious corrosion to the stainless steel cell case and a thicker and looser surface film on Li anode. In conclusion, the key findings of this work emphasize that the salt chemistry is critically important for enhancing the interfacial stability of Li metal anode and should be carefully manipulated in the development of high performance Li metal batteries.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [3] ;  [4] ;  [2] ;  [2]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Southwest Petroleum Univ., Sichuan (China)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Beijing Univ. of Chemical Technology, Beijing (China)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Xiamen Univ., Fujian (China)
Publication Date:
Report Number(s):
PNNL-SA-128903
Journal ID: ISSN 1944-8244; TRN: US1800750
Grant/Contract Number:
AC02-05CH11231; AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Building Technologies Office (EE-5B); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Li metal batteries; dual-salt electrolyte; surface film; cathode electrolyte interphase; cycling stability; 36 MATERIALS SCIENCE
OSTI Identifier:
1414952
Alternate Identifier(s):
OSTI ID: 1415141