Impact of thickness of the solid electrolyte interphase (SEI) film on

the working efficiency of secondary ion batteries

Summary:
Solid electrolyte interphase (SEI) is a passivation layer formed on electrode surfaces from
decomposition products of electrolytes. The SEI permits transportation of Li+ and blocks
electrons in order to prevent further electrolyte decomposition and ensure continued
electrochemical reactions. The formation and growth mechanism of the nanometer thick SEI
films are yet to be completely understood because of their complex structure and lack of reliable
in situ experimental techniques. Significant advances in computational methods have made it
possible for predicting the model of fundamentals for SEI. Here, the main objective of my
project is to analyze the thickness of SEI film and therefore finding the optimum thickness of
SEI film for improving efficiency of Li-ion batteries. Simulation software Comsol Multiphysics
5.3a will be used for analyzing and finding the desired optimum thickness of SEI film. The
findings of this project will help us to comprehend a better understanding of the complex SEI for
the development of a highly efficient battery in the future.

Statement of problem:

The solid electrolyte interphase (SEI) is a protecting layer formed on the negative electrode of
Li-ion batteries due to electrolyte decomposition, mainly during the first cycle. Battery
performance, irreversible charge “loss”, rate capability, exfoliation of graphite and safety are
highly dependent on the quality of the SEI. Hence, understanding the actual nature and
composition of SEI is of prime interest to us. Now, if we understand the chemistry of the SEI
formation and the manner in which each component affects battery performance, SEI could be
tuned to improve battery performance. Moreover, as the SEI composition and contents are a
direct consequence of the electrolyte composition, thermodynamic instability and kinetic
reactivity of the electrolyte culminates into the SEI. Therefore, studying and analyzing the
effects of electrolytes on the structure of SEI and hence figuring out the optimum thickness of
the SEI film in Li-ion batteries will enable us to increase efficiency and enhance battery
performances in the future. The main objective of my project is to analyze the impacts of
changing thickness of SEI layer and hence the effect of optimum thickness of SEI film on the
performance of battery.
Background Literature Review:

As the global energy demand increases, developing energy storage systems with higher energy
densities is becoming more and more crucial. Rechargeable Li-ion batteries have been widely
utilized in portable electronics because of their high gravimetric energy storage and now are
being considered for critical applications such as heavy auto-motives and medical devices.
During the first charge of the Li-ion battery, the electrolyte decomposes at the surface of the
graphite anode and thus forming a film composed of inorganic and organic electrolyte
decomposition products, called the solid electrolyte interphase (SEI) [1]. It is known that this
layer provides kinetic stability to the electrolyte against further reduction in successive cycles
and thereby ensures good cyclability of the electrode but it leads to irreversible loss of Li and the
capacity of the battery [2-6]. Battery performance depends on the composition, thickness,
morphology, and compactness of the SEI significantly [7,8]. The properties of the SEI become
even more vital during cycling at high rates and at deeper depth of discharge. In particular,
during power cycling, large stresses build up in the electrode which leads to cracking of the SEI
films and graphite is again exposed to the electrolyte [9]. Growth of fresh SEI on the crack faces
leads to further loss of capacity [6]. Therefore understanding and analyzing the formation
mechanisms, composition, structure and mechanical and transport properties of the SEI is critical
for design of long-lived, high-performance batteries.

Models proposed by Peled et al. [10], Aurbach et al. [11,12], and Edstrom et al. [13,14] suggest
SEI to be a dense layer of inorganic components close to the anode, followed by a porous
organic or polymeric layer close to the electrolyte phase. From an experimental point of view, as
most of the characterization analysis of the SEI are carried out ex-situ, it is difficult to
understand with a high degree of certainty whether the structure of the SEI is influenced by the
artifacts of the measurement and processing techniques. Therefore detailed information of the
composition and morphology of the SEI are currently under debate. For example, Leifer et al.
very recently proposed an entirely new family of SEI products, which have not been identified in
prior work using XPS and FT-IR [15]. Given the experimental complexity in characterizing the
SEI, a natural question to ask is whether computational models can be used to address issues
regarding the composition and structure of the SEI.

It is suggested that the outer layer of the SEI layer, whose pores are filled with electrolyte,
controls the progress of SEI growth, and consequently the extent of capacity fade and internal
resistance rise. The outer layer can be a couple of order of magnitudes thicker than the inner
layer, while at the same time the outer layer is more vulnerable and unstable [16,17-19].
SEI growth is dependent on the electron current flow and lithium diffusion, which vary at
different locations in the electrode [20]. Thus A cell level physics-based SEI growth model is
essential for revealing this spatial distribution of SEI and evaluate its effect on cell performance.
Moreover, it is important to integrate the temperature effect in the cell-level model because it
directly influences the material properties such as diffusivity and side reaction rates.
Temperature is also of interest for the study of thermal runaway as it is closely related to the
safety of LIBs.
A good SEI should be a compact layer adhering well to the anode. It should be elastic and
flexible to accommodate non-uniform electrochemical behavior and active material breathing. At
present, there is no information on the mechanical properties as well as the optimum thickness of
the SEI film and how these properties are related to the composition of the electrolyte.

Research Gaps :
Based on the review of the literature the following gaps are present in the past research:

 Optimum thickness for SEI Layer in Li-ion batteries.

 Investigating the mechanical properties of SEI layer.
 Examining the composition and spatial distribution of reduction products in SEI film.
 Electrolytes required for optimum thickness of SEI Layer.
 Compositional structure of SEI layer for achieving optimum state.

List of Research Questions :

Based on the identified gap, my research question are as follows:

Question_1: What should be the thickness value of the SEI layer for optimum state of operation
in Li-ion batteries?

Question_2: What should be the components of electrolytes in order to achieve optimum

thickness in SEI layer?

Question_3: What should be the structural composition of SEI layer during optimum state of
operation?

Methodology and Project Planning :

Detailed below is the general methodology required to address the major components of this
project:

 After completing the literature review, I will start to gather data about the required
electrochemical parameters of Li-ion batteries. By going through the detailed research
papers based on electrochemical properties of Li-ion batteries, I hope to acquire the
necessary data required for this project. My supervisor has also agreed to provide me
with the data needed for this project.
  Once the necessary simulation data are collected, I will start focusing on developing an
electrochemical aging model on Comsol Multiphysics 5.3a. Producing a precise
aforementioned aging model is needed to verify and compare the simulation results.
 After developing an electrochemical aging model, I will start changing the
electrochemical parameters of Li-ion batteries and therefore observe the variation of
thickness of the SEI layers.
 After observing the variations of thickness of SEI layer, I will try to find the thickness of
the layer for maximum Li-ion propagation and minimum electron conduction at ideal
battery conditions. This thickness value will correspond to the optimum thickness of SEI
layer.

A detailed breakdown of the individual tasks which needs to be completed are shown in Table-1
Task Breakdown and Methodology below. Also the project Gantt chart with project tracker
highlighting the estimated completion time of the project has provided.

Table 1 Task Breakdown and Methodology

Task no. Action Methodology/ Description

1. Literature Review Producing a literature review

will give my project a good
starting point by summarizing
all the relevant works and
research already done on the
topic. This will permit me to
identify and gaps in the past
research and highlight the
direction I want for my project.

2. Project proposal This will permit me to start

solidifying the direction I want
to take my project based on the
gaps identified in the literature
review.

3. Collecting data By going through the detailed

research papers based on the
 topic, all necessary parameter
data will be acquired.

4. Developing simulation model With the help of Comsol

Multiphysics software, an
aging electrochemical
simulation model will be
developed.
5. Simulation with After developing an
electrochemical parameter electrochemical aging model,
data changing of electrochemical
parameters of Li-ion batteries
will be performed and
therefore the variation of
thickness of the SEI layers
will observed.

6. Analysis of simulated data After analyzing the simulated

data, the thickness of the
layer for maximum Li-ion
propagation and minimum
electron conduction will be
found.
7. Formulate recommendations After finding the optimum
thickness of SEI layer, the
effect of it will be observed
on battery performance and
therefore formulating
recommendations based on
project findings.

Gantt Chart with Project Tracker :

Project Name: Impact of thickness of the solid electrolyte interphase (SEI) film on the
working efficiency of secondary ion batteries
ID Task Task Name Duration Start Finish Predecessors
Mode 4/11/19 6/21/19 9/1/20 11/11/20 1/21/20 4/1/20
1 Professional 64.19 days 8/20 11/15
Advanced
Engineering Project
Part-A
2 Literature Review 22.19 days 8/20 9/18

3 Data collection for 12.19 days 9/21 10/6

Simulation
parameters
4 Developing 16.19 days 9/25 10/16
Simulation Model
5 Project Report 3.19 days 10/17 10/19

Task Inactive Summary External Tasks

Split Manual Task External Milestone

Milestone Duration-only Deadline

Project: PEAP Gantts chart mod
Summary Manual Summary Rollup Progress
Date: 9/18
Project Summary Manual Summary Manual Progress

Inactive Task Start-only

Inactive Milestone Finish-only

Page 1
ID Task Task Name Duration Start Finish Predecessors
Mode 4/11/19 6/21/19 9/1/20 11/11/20 1/21/20 4/1/20
8 Professional 65.19 days 3/3 6/1
Advanced
Engineering Project
Part-B
9 Simulation with 35.19 days 3/3 4/20
obtained
electro-chemical data

10 Analysis of simulated 22.19 days 4/21 5/20

data
11 Formulate 5.19 days 5/21 5/27
recommendations
12 Preparing for final 3.19 days 5/28 6/1
project report and
presentation

Task Inactive Summary External Tasks

Split Manual Task External Milestone

Milestone Duration-only Deadline

Project: PEAP Gantts chart mod
Summary Manual Summary Rollup Progress
Date: 9/18
Project Summary Manual Summary Manual Progress

Inactive Task Start-only

Inactive Milestone Finish-only

Page 2
References:

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(2008) A442–A447.

[4] E. Markervich, G. Salitra, M.D. Levi, D. Aurbach, J. Power Sources 146 (2005) 146–150.

[5] D. Aurbach, B. Markovsky, I. Weissman, E. Levi, Y. Ein-Eli, Electrochim. Acta 45 (1999)

67–86.

[6] J. Vetter, P. Novak, M.R. Wagner, C. Veit, K.-C. Moller, J.O. Besenhard, M. Winter, M.
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[7] P.B. Balbuena, Y. Wang, Lithium-Ion Batteries: Solid–Electrolyte Interphase, Imperial

College Press, London, 2004.

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[15] N. Leifer, M.C. Smart, G.K.S. Prakash, L. Gonzalez, L. Sanchez, K.A. Smith, P. Bhalla,
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[16] A.M. Andersson, A. Henningson, H. Siegbahn, U. Jansson, K. Edstr€om, J. Power Sources

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141 (1994) 603e611.
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[20] M. Safari, M. Morcrette, A. Teyssot, C. Delacourt, J. Electrochem. Soc. 156 (2009)

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