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Role of Solution Structure in Solid Electrolyte Interphase Formation on Graphite with LiPF 6 in Propylene Carbonate

Journal Article · · Journal of Physical Chemistry. C
DOI:https://doi.org/10.1021/jp409765w· OSTI ID:1395010
 [1];  [2];  [1];  [1];  [1];  [1]
  1. University of Rhode Island, Kingston, Rhode Island 02881, United States
  2. Argonne National Laboratory, Argonne, Illinois 60438, United States
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An investigation of the interrelationship of cycling performance, solution structure, and electrode surface film structure has been conducted for electrolytes composed of different concentrations of LiPF6 in propylene carbonate (PC) with a binderfree (BF) graphite electrode. Varying the concentration of LiPF6 changes the solution structure, altering the predominant mechanism of electrolyte reduction at the electrode interface. The change in mechanism results in a change in the structure of the solid electrolyte interface (SEI) and the reversible cycling of the cell. At low concentrations of LiPF6 in PC (1.2 M), electrochemical cycling and cyclic voltammetry (CV) of BF graphite electrodes reveal continuous electrolyte reduction and no lithiation/delithiation of the graphite. The solution structure is dominated by solvent-separated ion pairs (Li+(PC)4// PF6 -), and the primary reduction product of the electrolyte is lithium propylene dicarbonate (LPDC). At high concentrations of LiPF6 in PC (3.0-3.5 M), electrochemical cycling and CV reveal reversible lithiation/delithiation of the graphite electrode. The solution structure is dominated by contact ion pairs (Li+(PC)3PF6 -), and the primary reduction product of the electrolyte is LiF.
Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
DOE Contract Number:
AC02-06CH11357
OSTI ID:
1395010
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 48 Vol. 117; ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

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