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Electrolyte Role in SEI Evolution at Si in the Pre-lithiation Stage vs the Post-lithiation Stage

Journal Article · · Journal of the Electrochemical Society
 [1];  [2];  [2];  [1]
  1. University of Massachusetts, Boston, MA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
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The formation and evolution of the dynamic solid electrolyte interphase (SEI) at the Si anode/electrolyte interface are yet to be completely understood to solve irreversible capacity loss and increase battery cycle life. Herein, the evolution of SEI and its dynamic properties at the Si anode/electrolyte interface are investigated in two electrolyte systems, a 1.2 M LiPF6 in EC: EMC 3:7 (wt%) electrolyte (referred to as Gen2) and a 1.2 M LiTFSI in EC: EMC 3:7 (wt%) electrolyte (referred to as LiTFSI). Two lithiation stages are studied: the pre-lithiation (pre-Li) SEI stage and the post-lithiation (post-Li) stage. Findings reveal at the pre-Li, SEI formation starts at an early potential and contributes to the greater mass gain in the Si/Gen2, and it is dominated by the formation of a non-uniform F- and P-rich layer in Si/Gen2, in contrast to a homogeneous F- and C-containing layer at the Si/LiTFSI interphase. The initially formed SEI in LiTFSI further benefits the charge transfer kinetics. At the post-Li stage, a more substantial SEI evolution is observed at Si/LiTFSI. This paper offers a foundational understanding of the SEI dynamic evolution with electrolyte dependence. Findings from this report offer important insights into solving the complex SEI stability issues on Si.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); National Science Foundation (NSF); University of Massachusetts, Boston, MA (United States)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1962414
Journal Information:
Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 2 Vol. 170; ISSN 0013-4651
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
NMR
SEI
battery
silicon
state of charge