Abstract
The performance of lithium-ion batteries (LIB) using organic electrolytes strongly depends on the formation of a stable solid electrolyte interphase (SEI) film. Elucidating the dynamic evolution and spatial composition of the SEI can be very useful to study the stability of SEI components and help optimize the formation cycles of LIB. We propose a classical molecular dynamics simulation protocol for predicting the first stages of SEI formation using a reaction method involving the decomposition of EC and LiPF6 molecules in the electrolyte. We accelerate the formation of SEI components near the anode surface by increasing the probability of reactions, implemented through a geometry matching scheme, followed by a force-field reconfiguration. We observe the formation of gases (C2H4), inorganic (Li2CO3 and LiF) and organic (LEDC) components. This protocol shows promise to be able to evaluate the effects of varying electrolyte compositions and additives on SEI layer structure and composition.
| Original language | English |
|---|---|
| Pages (from-to) | 18588-18596 |
| Number of pages | 9 |
| Journal | Journal of Physical Chemistry C |
| Volume | 125 |
| Issue number | 34 |
| DOIs | |
| State | Published - Sep 2 2021 |
Funding
This work is supported by the U.S. Department of Energy Vehicle Technologies Office and was carried out at Oak Ridge National Laboratory under Contract No. DE-AC05-00OR22725 with UT Battelle, LLC. This research used resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. We gratefully acknowledge Hetal D. Patel and Kara D. Fong for the fruitful discussion.
