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Title: Insights into the Li Intercalation and SEI Formation on LiSi Nanoclusters

Journal Article · · Journal of the Electrochemical Society
 [1];  [1];  [2]
  1. Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering
  2. Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering, Department of Materials Science and Engineering, and Department of Chemistry
+ Show Author Affiliations

We report a first-principles atomic level assessment of the lithiation and reactivity of pre-lithiated Si clusters. Density functional theory formation energy calculations reveal that the pre-lithiated Li16Si16 cluster exposed to two different Li fluxes can store Li between the concentrations of Li2.5Si and Li3.5Si. This increase in storage capacity is attributed to the start of an amorphization process in the cluster, and more importantly these results show that the intercalation reaction can be controlled by the flux of the Li-ions. However, in a real battery, the lithiation of the anode occurs simultaneously to the electrode-electrolyte reactions. Here we simulate the solid-electrolyte interphase (SEI) formation and simultaneous lithiation of a Li16Si16 cluster in contact with two different electrolyte solutions: one with pure ethylene carbonate (EC), and another with a 1 M solution of LiPF6 in EC. Our ab initio molecular dynamics simulations show that the solvent and salt are decomposed leading to the initial stages of the SEI layer formation and large part of the added Li becomes part of the SEI. Interestingly, the pure EC solution results in lower storage capacity and higher reactivity, whereas the presence of the salt causes the opposite effect: higher lithiation and reduced reactivity.

Research Organization:
Texas A & M Univ., College Station, TX (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Vehicle Technologies Office (VTO)
Grant/Contract Number:
EE0007766
OSTI ID:
1430637
Alternate ID(s):
OSTI ID: 1868489
Journal Information:
Journal of the Electrochemical Society, Vol. 164, Issue 11; ISSN 0013-4651
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

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  • Ramos-Sanchez, G.; Soto, F. A.; Martinez de la Hoz, J. M.
  • Journal of Electrochemical Energy Conversion and Storage, Vol. 13, Issue 3 https://doi.org/10.1115/1.4034412
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Cited By (2)

Ab Initio-Based Structural and Thermodynamic Aspects of the Electrochemical Lithiation of Silicon Nanoparticles journal December 2019
Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries journal March 2018

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Related Subjects

25 ENERGY STORAGE
36 MATERIALS SCIENCE
ab initio molecular dynamics
density functional theory
irreversible capacity
lithiation
SEI
silicon anodes