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Title: The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling

Abstract

An in-depth review is presented on the science of lithium-ion battery (LIB) solid electrolyte interphase (SEI) formation on the graphite anode, including structure, morphology, chemical composition, electrochemistry, formation mechanism, and LIB formation cycling. During initial operation of LIBs, the SEI layer forms on the graphite surfaces, the most commonly used anode material, due to side reactions with the electrolyte solvent/salt at low electro-reduction potentials. It is accepted that the SEI layer is essential to the long-term performance of LIBs, and it also has an impact on its initial capacity loss, self-discharge characteristics, cycle life, rate capability, and safety. While the presence of the anode SEI layer is vital, it is difficult to control its formation and growth, as the chemical composition, morphology, and stability depend on several factors. These factors include the type of graphite, electrolyte composition, electrochemical conditions, and cell temperature. Thus, SEI layer formation and electrochemical stability over long-term operation should be a primary topic of future investigation in the development of LIB technology. We review the progression of knowledge gained about the anode SEI, from its discovery in 1979 to the current state of understanding, and covers its formation process, differences in the chemical and structural makeupmore » when cell materials and components are varied, methods of characterization, and associated reactions with the liquid electrolyte phase. It also discusses the relationship of the SEI layer to the LIB formation step, which involves both electrolyte wetting and subsequent slow charge-discharge cycles to grow the SEI.« less

Authors:
; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). National Transportation Research Center (NTRC); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Manufacturing Demonstration Facility (MDF)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1248056
Alternate Identifier(s):
OSTI ID: 1248766
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Published Article
Journal Name:
Carbon
Additional Journal Information:
Journal Name: Carbon Journal Volume: 105 Journal Issue: C; Journal ID: ISSN 0008-6223
Publisher:
Elsevier
Country of Publication:
United Kingdom
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; SEI; review

Citation Formats

An, Seong Jin, Li, Jianlin, Daniel, Claus, Mohanty, Debasish, Nagpure, Shrikant, and Wood, III, David L. The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling. United Kingdom: N. p., 2016. Web. doi:10.1016/j.carbon.2016.04.008.
An, Seong Jin, Li, Jianlin, Daniel, Claus, Mohanty, Debasish, Nagpure, Shrikant, & Wood, III, David L. The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling. United Kingdom. https://doi.org/10.1016/j.carbon.2016.04.008
An, Seong Jin, Li, Jianlin, Daniel, Claus, Mohanty, Debasish, Nagpure, Shrikant, and Wood, III, David L. Mon . "The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling". United Kingdom. https://doi.org/10.1016/j.carbon.2016.04.008.
@article{osti_1248056,
title = {The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling},
author = {An, Seong Jin and Li, Jianlin and Daniel, Claus and Mohanty, Debasish and Nagpure, Shrikant and Wood, III, David L.},
abstractNote = {An in-depth review is presented on the science of lithium-ion battery (LIB) solid electrolyte interphase (SEI) formation on the graphite anode, including structure, morphology, chemical composition, electrochemistry, formation mechanism, and LIB formation cycling. During initial operation of LIBs, the SEI layer forms on the graphite surfaces, the most commonly used anode material, due to side reactions with the electrolyte solvent/salt at low electro-reduction potentials. It is accepted that the SEI layer is essential to the long-term performance of LIBs, and it also has an impact on its initial capacity loss, self-discharge characteristics, cycle life, rate capability, and safety. While the presence of the anode SEI layer is vital, it is difficult to control its formation and growth, as the chemical composition, morphology, and stability depend on several factors. These factors include the type of graphite, electrolyte composition, electrochemical conditions, and cell temperature. Thus, SEI layer formation and electrochemical stability over long-term operation should be a primary topic of future investigation in the development of LIB technology. We review the progression of knowledge gained about the anode SEI, from its discovery in 1979 to the current state of understanding, and covers its formation process, differences in the chemical and structural makeup when cell materials and components are varied, methods of characterization, and associated reactions with the liquid electrolyte phase. It also discusses the relationship of the SEI layer to the LIB formation step, which involves both electrolyte wetting and subsequent slow charge-discharge cycles to grow the SEI.},
doi = {10.1016/j.carbon.2016.04.008},
journal = {Carbon},
number = C,
volume = 105,
place = {United Kingdom},
year = {Mon Aug 01 00:00:00 EDT 2016},
month = {Mon Aug 01 00:00:00 EDT 2016}
}

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https://doi.org/10.1016/j.carbon.2016.04.008

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Influence of morphology on electrochemical and capacity performance of open-porous structured electrodes
journal, January 2020


Enhanced lithium storage capability enabled by metal nickel dotted NiO–graphene composites
journal, September 2018


Toward Low-Cost, High-Energy Density, and High-Power Density Lithium-Ion Batteries
journal, June 2017


Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions
journal, February 2018

  • Chaudhari, Mangesh I.; Muralidharan, Ajay; Pratt, Lawrence R.
  • Topics in Current Chemistry, Vol. 376, Issue 2
  • DOI: 10.1007/s41061-018-0187-2

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries
journal, March 2018


Chitosan complements entrapment of silicon inside nitrogen doped carbon to improve and stabilize the capacity of Li-ion batteries
journal, March 2019


Electrocatalytic transformation of HF impurity to H2 and LiF in lithium-ion batteries
journal, April 2018


Running out of lithium? A route to differentiate between capacity losses and active lithium losses in lithium-ion batteries
journal, January 2017

  • Holtstiege, Florian; Wilken, Andrea; Winter, Martin
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 38
  • DOI: 10.1039/c7cp05405j

A highly stabilized nickel-rich cathode material by nanoscale epitaxy control for high-energy lithium-ion batteries
journal, January 2018

  • Kim, Junhyeok; Ma, Hyunsoo; Cha, Hyungyeon
  • Energy & Environmental Science, Vol. 11, Issue 6
  • DOI: 10.1039/c8ee00155c

Probing microstructure and electrolyte concentration dependent cell chemistry via operando small angle neutron scattering
journal, January 2019

  • Jafta, Charl J.; Sun, Xiao-Guang; Veith, Gabriel M.
  • Energy & Environmental Science, Vol. 12, Issue 6
  • DOI: 10.1039/c8ee02703j

Tungsten oxide nanorod architectures as 3D anodes in binder-free lithium-ion batteries
journal, January 2019

  • Herdt, Tim; Deckenbach, Daniel; Bruns, Michael
  • Nanoscale, Vol. 11, Issue 2
  • DOI: 10.1039/c8nr07636g

Ex situ solid electrolyte interphase synthesis via radiolysis of Li-ion battery anode–electrolyte system for improved coulombic efficiency
journal, January 2018

  • Varenne, Fanny; Alper, John P.; Miserque, Frédéric
  • Sustainable Energy & Fuels, Vol. 2, Issue 9
  • DOI: 10.1039/c8se00257f

Three-dimensional carbon/ZnO nanomembrane foam as an anode for lithium-ion battery with long-life and high areal capacity
journal, January 2018

  • Zhao, Yuting; Huang, Gaoshan; Li, Yalan
  • Journal of Materials Chemistry A, Vol. 6, Issue 16
  • DOI: 10.1039/c8ta00940f

Dual carbon-protected metal sulfides and their application to sodium-ion battery anodes
journal, January 2018

  • Zhu, Xinxin; Liu, Dan; Zheng, Dong
  • Journal of Materials Chemistry A, Vol. 6, Issue 27
  • DOI: 10.1039/c8ta03444c

Improving the structure stabilization of red phosphorus anodes via the shape memory effect of a Ni–Ti alloy for high-performance sodium ion batteries
journal, January 2019

  • Wang, Yingtao; Yang, Xiaodan; Zhao, Chenyang
  • Chemical Communications, Vol. 55, Issue 32
  • DOI: 10.1039/c9cc00024k

On principal features of organic electrolyte molecules in lithium ion battery performance
journal, January 2019

  • Tsuneda, Takao; Tateyama, Yoshitaka
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 41
  • DOI: 10.1039/c9cp03980e

Intercalation chemistry of graphite: alkali metal ions and beyond
journal, January 2019

  • Li, Yuqi; Lu, Yaxiang; Adelhelm, Philipp
  • Chemical Society Reviews, Vol. 48, Issue 17
  • DOI: 10.1039/c9cs00162j

Thermodynamic insights into the free energy of the processes in lithium iron phosphate batteries
journal, January 2019

  • Priyadarshini, C. Hepsibah; Harinipriya, S.; Sudha, V.
  • New Journal of Chemistry, Vol. 43, Issue 35
  • DOI: 10.1039/c9nj03041g

Enhanced high rate capability of Li intercalation in planar and edge defect-rich MoS 2 nanosheets
journal, January 2019

  • Budumuru, Akshay Kumar; Rakesh, Benadict; Sudakar, Chandran
  • Nanoscale, Vol. 11, Issue 18
  • DOI: 10.1039/c9nr02043h

Self-templated construction of 1D NiMo nanowires via a Li electrochemical tuning method for the hydrogen evolution reaction
journal, January 2019

  • Huang, Dekang; Li, Shu; Luo, Yanzhu
  • Nanoscale, Vol. 11, Issue 41
  • DOI: 10.1039/c9nr05311e

Designing superior solid electrolyte interfaces on silicon anodes for high-performance lithium-ion batteries
journal, January 2019

  • Zhang, Yaguang; Du, Ning; Yang, Deren
  • Nanoscale, Vol. 11, Issue 41
  • DOI: 10.1039/c9nr05748j

Deciphering the lithium ion movement in lithium ion batteries: determination of the isotopic abundances of 6 Li and 7 Li
journal, January 2019

  • Diehl, Marcel; Evertz, Marco; Winter, Martin
  • RSC Advances, Vol. 9, Issue 21
  • DOI: 10.1039/c9ra02312g

Silica from diatom frustules as anode material for Li-ion batteries
journal, January 2019

  • Norberg, Andreas Nicolai; Wagner, Nils Peter; Kaland, Henning
  • RSC Advances, Vol. 9, Issue 70
  • DOI: 10.1039/c9ra07271c

Mechanistic insight into the improved Li ion conductivity of solid polymer electrolytes
journal, January 2019

  • Patra, Sudeshna; Thakur, Pallavi; Soman, Bhaskar
  • RSC Advances, Vol. 9, Issue 66
  • DOI: 10.1039/c9ra08003a

Carbon-based artificial SEI layers for aqueous lithium-ion battery anodes
journal, January 2020

  • Subramanya, Usha; Chua, Charleston; He Leong, Victor Gin
  • RSC Advances, Vol. 10, Issue 2
  • DOI: 10.1039/c9ra08268a

An all solid-state Li ion battery composed of low molecular weight crystalline electrolyte
journal, January 2020

  • Joshi, Prerna; Vedarajan, Raman; Sheelam, Anjaiah
  • RSC Advances, Vol. 10, Issue 15
  • DOI: 10.1039/c9ra09559d

Understanding the electrochemical potential and diffusivity of MnO/C nanocomposites at various charge/discharge states
journal, January 2019

  • Liu, Chaofeng; Fu, Haoyu; Pei, Yanyan
  • Journal of Materials Chemistry A, Vol. 7, Issue 13
  • DOI: 10.1039/c9ta00056a

Real-time monitoring of stress development during electrochemical cycling of electrode materials for Li-ion batteries: overview and perspectives
journal, January 2019

  • Jangid, Manoj K.; Mukhopadhyay, Amartya
  • Journal of Materials Chemistry A, Vol. 7, Issue 41
  • DOI: 10.1039/c9ta06474e

Ultrathin Al foils to fabricate dendrite-free Li–Al anodes
journal, January 2019

  • Wu, Lan; He, Guang; Ding, Yi
  • Journal of Materials Chemistry A, Vol. 7, Issue 44
  • DOI: 10.1039/c9ta09464d

A materials perspective on magnesium-ion-based solid-state electrolytes
journal, January 2020

  • Jaschin, Prem Wicram; Gao, Yirong; Li, Yao
  • Journal of Materials Chemistry A, Vol. 8, Issue 6
  • DOI: 10.1039/c9ta11729f

Heat Generation and Thermal Transport in Lithium-Ion Batteries: A Scale-Bridging Perspective
journal, November 2018


Creation of nanosized holes in graphene planes for improvement of rate capability of lithium-ion batteries
journal, February 2018


Free-anchored Nb 2 O 5 @graphene networks for ultrafast-stable lithium storage
journal, March 2018


Flexible fiber-shaped energy storage devices: principles, progress, applications and challenges
journal, February 2018


Active formation of Li-ion batteries and its effect on cycle life
journal, August 2019

  • Pathan, Tanveerkhan S.; Rashid, Muhammad; Walker, Marc
  • Journal of Physics: Energy, Vol. 1, Issue 4
  • DOI: 10.1088/2515-7655/ab2e92

Atomic structure of sensitive battery materials and interfaces revealed by cryo–electron microscopy
journal, October 2017


Controlling Expansion in Lithium Manganese Oxide Composite Electrodes via Surface Modification
journal, January 2019

  • Çapraz, Ö. Ö.; Rajput, S.; Bassett, K. L.
  • Journal of The Electrochemical Society, Vol. 166, Issue 12
  • DOI: 10.1149/2.0021912jes

Design and Demonstration of Three-Electrode Pouch Cells for Lithium-Ion Batteries
journal, January 2017

  • An, Seong Jin; Li, Jianlin; Daniel, Claus
  • Journal of The Electrochemical Society, Vol. 164, Issue 7
  • DOI: 10.1149/2.0031709jes

Effect of Formation Potentials on Gassing of LiMn 2 O 4 //Li 4 Ti 5 O 12 /C Batteries
journal, November 2018

  • Wen, Lei; Wu, Zeyi; Zhao, Peng
  • Journal of The Electrochemical Society, Vol. 166, Issue 3
  • DOI: 10.1149/2.0081903jes

Influence of the Electrolyte Quantity on Lithium-Ion Cells
journal, January 2019

  • Günter, Florian J.; Burgstaller, Clemens; Konwitschny, Fabian
  • Journal of The Electrochemical Society, Vol. 166, Issue 10
  • DOI: 10.1149/2.0121910jes

A Physics-Based Model Capacity Fade Analysis of LiMn 2 O 4 /Graphite Cell at Different Temperatures
journal, November 2018

  • Appiah, Williams Agyei; Ryou, Myung-Hyun; Lee, Yong Min
  • Journal of The Electrochemical Society, Vol. 166, Issue 3
  • DOI: 10.1149/2.0161903jes

Calendar Aging and Gas Generation in Commercial Graphite/NMC-LMO Lithium-Ion Pouch Cell
journal, January 2017

  • Mao, Z.; Farkhondeh, M.; Pritzker, M.
  • Journal of The Electrochemical Society, Vol. 164, Issue 14
  • DOI: 10.1149/2.0241714jes

Mechanical and Electronic Stabilization of Solid Electrolyte Interphase with Sulfite Additive for Lithium Metal Batteries
journal, January 2019

  • Xu, Jiagang; Tian, Hong-Kang; Qi, Ji
  • Journal of The Electrochemical Society, Vol. 166, Issue 14
  • DOI: 10.1149/2.0331914jes

Predicting High-Temperature Decomposition of Lithiated Graphite: Part I. Review of Phenomena and a Comprehensive Model
journal, January 2018

  • Shurtz, Randy C.; Engerer, Jeffrey D.; Hewson, John C.
  • Journal of The Electrochemical Society, Vol. 165, Issue 16
  • DOI: 10.1149/2.0541816jes

Effects of Ultraviolet Light Treatment in Ambient Air on Lithium-Ion Battery Graphite and PVDF Binder
journal, January 2019

  • An, Seong Jin; Li, Jianlin; Daniel, Claus
  • Journal of The Electrochemical Society, Vol. 166, Issue 6
  • DOI: 10.1149/2.0591906jes

Electrochemistry-Mechanics Coupling in Intercalation Electrodes
journal, January 2018

  • Kotak, Nihar; Barai, Pallab; Verma, Ankit
  • Journal of The Electrochemical Society, Vol. 165, Issue 5
  • DOI: 10.1149/2.0621805jes

Controlled Prelithiation of PbS to Pb/Li 2 S for High Initial Coulombic Efficiency in Lithium Ion Batteries
journal, January 2019

  • Guo, Alan; Chen, Eric; Heller, Adam
  • Journal of The Electrochemical Society, Vol. 166, Issue 10
  • DOI: 10.1149/2.0641910jes

Influence of Current Density on Graphite Anode Failure in Lithium-Ion Batteries
journal, January 2019

  • Zhang, Pengcheng; Yuan, Tao; Pang, Yuepeng
  • Journal of The Electrochemical Society, Vol. 166, Issue 3
  • DOI: 10.1149/2.0701903jes

Means of Using Cyclic Voltammetry to Rapidly Design a Stable DMC-Based Electrolyte for Na-Ion Batteries
journal, January 2019

  • Cometto, Claudio; Yan, Guochun; Mariyappan, Sathiya
  • Journal of The Electrochemical Society, Vol. 166, Issue 15
  • DOI: 10.1149/2.0721915jes

Visualized Pulverization via Ex Situ Analyses: Nickel Sulfide Anode Caged in a Hierarchical Carbon
journal, January 2019

  • Park, Jae Hyun; Lee, Jae W.
  • Journal of The Electrochemical Society, Vol. 166, Issue 6
  • DOI: 10.1149/2.1071904jes

Mixed Mode Growth Model for the Solid Electrolyte Interface (SEI)
journal, January 2019

  • Kamyab, Niloofar; Weidner, John W.; White, Ralph E.
  • Journal of The Electrochemical Society, Vol. 166, Issue 2
  • DOI: 10.1149/2.1101902jes

Amount of Free Liquid Electrolyte in Commercial Large Format Prismatic Li-Ion Battery Cells
journal, January 2019

  • Lebedeva, Natalia P.; Persio, Franco Di; Kosmidou, Theodora
  • Journal of The Electrochemical Society, Vol. 166, Issue 4
  • DOI: 10.1149/2.1151904jes

Structural and Electrochemical Characterization of Thin Film Li 2 MoO 3 Electrodes
journal, January 2019

  • Self, Ethan C.; Zhang, Yiman; Kercher, Andrew K.
  • Journal of The Electrochemical Society, Vol. 166, Issue 6
  • DOI: 10.1149/2.1161904jes

Interrelation between Redox Molecule Transport and Li + Ion Transport across a Model Solid Electrolyte Interphase Grown on a Glassy Carbon Electrode
journal, January 2017

  • Kranz, T.; Kranz, S.; Miß, V.
  • Journal of The Electrochemical Society, Vol. 164, Issue 14
  • DOI: 10.1149/2.1171714jes

The Influence of Anode/Cathode Capacity Ratio on Cycle Life and Potential Variations of Lithium-Ion Capacitors
journal, January 2019

  • Naderi, R.; Shellikeri, A.; Hagen, M.
  • Journal of The Electrochemical Society, Vol. 166, Issue 12
  • DOI: 10.1149/2.1171912jes

Assessment of Li-Inventory in Cycled Si-Graphite Anodes Using LiFePO 4 as a Diagnostic Cathode
journal, January 2018

  • Dose, Wesley M.; Maroni, Victor A.; Piernas-Muñoz, Maria Jose
  • Journal of The Electrochemical Society, Vol. 165, Issue 10
  • DOI: 10.1149/2.1271810jes

Advancing Lithium- and Manganese-Rich Cathodes through a Combined Electrolyte Additive/Surface Treatment Strategy
journal, January 2019

  • Gutierrez, Arturo; He, Meinan; Yonemoto, Bryan T.
  • Journal of The Electrochemical Society, Vol. 166, Issue 16
  • DOI: 10.1149/2.1281915jes

Review—SEI: Past, Present and Future
journal, January 2017

  • Peled, E.; Menkin, S.
  • Journal of The Electrochemical Society, Vol. 164, Issue 7
  • DOI: 10.1149/2.1441707jes

Pre-Lithiation Strategies for Rechargeable Energy Storage Technologies: Concepts, Promises and Challenges
journal, January 2018


A Post-Mortem Study of Stacked 16 Ah Graphite//LiFePO4 Pouch Cells Cycled at 5 °C
journal, May 2019

  • Moretti, Arianna; Carvalho, Diogo Vieira; Ehteshami, Niloofar
  • Batteries, Vol. 5, Issue 2
  • DOI: 10.3390/batteries5020045

Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries
journal, January 2020

  • Teichert, Philipp; Eshetu, Gebrekidan Gebresilassie; Jahnke, Hannes
  • Batteries, Vol. 6, Issue 1
  • DOI: 10.3390/batteries6010008

Capacity Decay Mechanism of the LCO + NMC532/Graphite Cells Combined with Post-Mortem Technique
journal, August 2017

  • Zhang, Linjing; Jiang, Jiuchun; Zhang, Weige
  • Energies, Vol. 10, Issue 8
  • DOI: 10.3390/en10081147

New Fe2O3-Clay@C Nanocomposite Anodes for Li-Ion Batteries Obtained by Facile Hydrothermal Processes
journal, October 2018

  • Alonso-Domínguez, Daniel; Pico, María; Álvarez-Serrano, Inmaculada
  • Nanomaterials, Vol. 8, Issue 10
  • DOI: 10.3390/nano8100808

POSS-Derived Synthesis and Full Life Structural Analysis of Si@C as Anode Material in Lithium Ion Battery
journal, March 2019