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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 Lab. (ORNL), Oak Ridge, TN (United States). National Transportation Research Center (NTRC); Oak Ridge National Lab. (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. https://doi.org/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 = {2016},
month = {8}
}

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

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    journal, March 2019

    • Mandli, Aravinda R.; Kaushik, Anshul; Patil, Rajkumar S.
    • International Journal of Energy Research, Vol. 43, Issue 6
    • DOI: 10.1002/er.4397

    Ab initio simulations of liquid electrolytes for energy conversion and storage
    journal, October 2018

    • Pham, Tuan Anh
    • International Journal of Quantum Chemistry, Vol. 119, Issue 1
    • DOI: 10.1002/qua.25795

    Niobium‐Based Oxides Toward Advanced Electrochemical Energy Storage: Recent Advances and Challenges
    journal, February 2019


    Key Aspects of Lithium Metal Anodes for Lithium Metal Batteries
    journal, March 2019


    Investigation of various layered lithium ion battery cathode materials by plasma- and X-ray-based element analytical techniques
    journal, October 2018

    • Evertz, Marco; Kasnatscheew, Johannes; Winter, Martin
    • Analytical and Bioanalytical Chemistry, Vol. 411, Issue 1
    • DOI: 10.1007/s00216-018-1441-8

    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