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Title: Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries

Abstract

Morphological defects contribute to chronic and acute failures of batteries. The development of these morphological defects entails the multiscale chemo-mechanical coupling associated with internal mechanical stress. The mechanical stress, caused by anisotropic structural, chemical and state of charge (SOC) heterogeneities, is released through crack formation, undermining the continuous diffusion pathways of electrons and ions and creating fresh surfaces for electrode–electrolyte side reactions. The understanding of chemomechanical interplay has remained at the descriptive level, thus, the quantification or model to fingerprint these processes is highly desired. Herein, we systematically investigate the mesoscale morphological defects within LiNi0.6Mn0.2Co0.2O2 secondary particles that have gone through fast-charging conditions. With the advanced synchrotron X-ray tomography, we nondestructively pierce the internal volume of secondary particles and quantify the morphological outcomes of the crack formation, such as porosity and internal surface area. We then develop a numerical model to predict the crack-induced diffusion deterrent of electrons and lithium ions. The mismatch between the local ionic and electronic conductivity can lead to highly heterogeneous SOC distribution in secondary particles, which exponentially deteriorates as the current density increases. In conclusion, our incisive investigation of chemomechanical interplay and fast-charging can inform a knowledge base to accelerate the discovery of advanced materialsmore » that are resilient against chemomechanical failures.« less

Authors:
 [1];  [2];  [2];  [3];  [4];  [5];  [4];  [6]; ORCiD logo [3]; ORCiD logo [2];  [4]
  1. Nanjing University of Science and Technology, Jiangsu (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  3. CAS, Beijing (China)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Nanjing University of Science and Technology, Jiangsu (China)
  6. Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1490861
Alternate Identifier(s):
OSTI ID: 1637160
Grant/Contract Number:  
2017YFB0102004; 51822211; DMR-1832613; DMR-1832707; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 53; Journal Issue: C; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Cathode; Li-ion battery; Crack; Transmission X-ray microscopy; Fast charging; Chemomechanical interplay

Citation Formats

Xia, Sihao, Mu, Linqin, Xu, Zhengrui, Wang, Junyang, Wei, Chenxi, Liu, Lei, Pianetta, Piero, Zhao, Kejie, Yu, Xiqian, Lin, Feng, and Liu, Yijin. Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries. United States: N. p., 2018. Web. https://doi.org/10.1016/j.nanoen.2018.09.051.
Xia, Sihao, Mu, Linqin, Xu, Zhengrui, Wang, Junyang, Wei, Chenxi, Liu, Lei, Pianetta, Piero, Zhao, Kejie, Yu, Xiqian, Lin, Feng, & Liu, Yijin. Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries. United States. https://doi.org/10.1016/j.nanoen.2018.09.051
Xia, Sihao, Mu, Linqin, Xu, Zhengrui, Wang, Junyang, Wei, Chenxi, Liu, Lei, Pianetta, Piero, Zhao, Kejie, Yu, Xiqian, Lin, Feng, and Liu, Yijin. Sat . "Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries". United States. https://doi.org/10.1016/j.nanoen.2018.09.051. https://www.osti.gov/servlets/purl/1490861.
@article{osti_1490861,
title = {Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries},
author = {Xia, Sihao and Mu, Linqin and Xu, Zhengrui and Wang, Junyang and Wei, Chenxi and Liu, Lei and Pianetta, Piero and Zhao, Kejie and Yu, Xiqian and Lin, Feng and Liu, Yijin},
abstractNote = {Morphological defects contribute to chronic and acute failures of batteries. The development of these morphological defects entails the multiscale chemo-mechanical coupling associated with internal mechanical stress. The mechanical stress, caused by anisotropic structural, chemical and state of charge (SOC) heterogeneities, is released through crack formation, undermining the continuous diffusion pathways of electrons and ions and creating fresh surfaces for electrode–electrolyte side reactions. The understanding of chemomechanical interplay has remained at the descriptive level, thus, the quantification or model to fingerprint these processes is highly desired. Herein, we systematically investigate the mesoscale morphological defects within LiNi0.6Mn0.2Co0.2O2 secondary particles that have gone through fast-charging conditions. With the advanced synchrotron X-ray tomography, we nondestructively pierce the internal volume of secondary particles and quantify the morphological outcomes of the crack formation, such as porosity and internal surface area. We then develop a numerical model to predict the crack-induced diffusion deterrent of electrons and lithium ions. The mismatch between the local ionic and electronic conductivity can lead to highly heterogeneous SOC distribution in secondary particles, which exponentially deteriorates as the current density increases. In conclusion, our incisive investigation of chemomechanical interplay and fast-charging can inform a knowledge base to accelerate the discovery of advanced materials that are resilient against chemomechanical failures.},
doi = {10.1016/j.nanoen.2018.09.051},
journal = {Nano Energy},
number = C,
volume = 53,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:

Citation Metrics:
Cited by: 14 works
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Figures / Tables:

Figure 1 Figure 1: X-ray micro and nano tomographic imaging of the battery electrode. Panels a and b illustrate the battery coin cells and their architectural structure. Panel c is the x-ray micro CT data of a small piece of cathode electrode. Panel d is the nano-resolution transmission x-ray microscopic mosaic imagemore » of a selected region on the electrode. Panels e-h are x-ray nano CT data of a few representative particles after fast cycling.« less

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Works referenced in this record:

Overcharge reaction of lithium-ion batteries
journal, August 2005


Operando Spectroscopic Microscopy of LiCoO2 Cathodes Outside Standard Operating Potentials
journal, September 2017


Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries
journal, March 2014

  • Lin, Feng; Markus, Isaac M.; Nordlund, Dennis
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4529

Utilizing Environmental Friendly Iron as a Substitution Element in Spinel Structured Cathode Materials for Safer High Energy Lithium-Ion Batteries
journal, December 2015

  • Hu, Enyuan; Bak, Seong-Min; Liu, Yijin
  • Advanced Energy Materials, Vol. 6, Issue 3
  • DOI: 10.1002/aenm.201501662

Assessment of the Wettability of Porous Electrodes for Lithium-Ion Batteries
journal, August 2004


Insitu nanotomography and operando transmission X-ray microscopy of micron-sized Ge particles
journal, January 2014

  • Weker, J. Nelson; Liu, N.; Misra, S.
  • Energy Environ. Sci., Vol. 7, Issue 8
  • DOI: 10.1039/C4EE01384K

Nanoscale Morphological and Chemical Changes of High Voltage Lithium–Manganese Rich NMC Composite Cathodes with Cycling
journal, July 2014

  • Yang, Feifei; Liu, Yijin; Martha, Surendra K.
  • Nano Letters, Vol. 14, Issue 8
  • DOI: 10.1021/nl502090z

Dissolution Mechanisms of LiNi 1/3 Mn 1/3 Co 1/3 O 2 Positive Electrode Material from Lithium-Ion Batteries in Acid Solution
journal, April 2018

  • Billy, Emmanuel; Joulié, Marion; Laucournet, Richard
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 19
  • DOI: 10.1021/acsami.8b01352

Modeling Battery Performance Due to Intercalation Driven Volume Change in Porous Electrodes
journal, July 2016


Oxygen Release Induced Chemomechanical Breakdown of Layered Cathode Materials
journal, April 2018


Propagation topography of redox phase transformations in heterogeneous layered oxide cathode materials
journal, July 2018


Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode
journal, June 2018


In Situ X-Ray Spectroscopy and Imaging of Battery Materials
journal, January 2011

  • Shearing, P.; Wu, Y.; Harris, S. J.
  • Interface magazine, Vol. 20, Issue 3
  • DOI: 10.1149/2.F03113if

In situ X-ray diffraction techniques as a powerful tool to study battery electrode materials
journal, July 2002


In situ X-ray diffraction and X-ray absorption studies of high-rate lithium-ion batteries
journal, January 2001


Mitigated phase transition during first cycle of a Li-rich layered cathode studied by in operando synchrotron X-ray powder diffraction
journal, January 2016

  • Song, Bohang; Day, Sarah J.; Sui, Tan
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 6
  • DOI: 10.1039/C5CP04801J

Synchrotron X-ray Analytical Techniques for Studying Materials Electrochemistry in Rechargeable Batteries
journal, September 2017


Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities
journal, January 2018

  • Rahman, Muhammad Mominur; Xu, Yahong; Cheng, Hao
  • Energy & Environmental Science, Vol. 11, Issue 9
  • DOI: 10.1039/C8EE00309B

Metal segregation in hierarchically structured cathode materials for high-energy lithium batteries
journal, January 2016


Intergranular Cracking as a Major Cause of Long-Term Capacity Fading of Layered Cathodes
journal, May 2017


Visualization and Quantification of Electrochemical and Mechanical Degradation in Li Ion Batteries
journal, October 2013


Understanding the initial irreversibility of metal sulfides for sodium-ion batteries via operando techniques
journal, January 2018


Probing Battery Electrochemistry with In Operando Synchrotron X-Ray Imaging Techniques
journal, March 2018


In Situ Atomic Force Microscopy of Lithiation and Delithiation of Silicon Nanostructures for Lithium Ion Batteries
journal, September 2013

  • Becker, Collin R.; Strawhecker, Kenneth E.; McAllister, Quinn P.
  • ACS Nano, Vol. 7, Issue 10
  • DOI: 10.1021/nn4037909

Fundamental degradation mechanisms of layered oxide Li-ion battery cathode materials: Methodology, insights and novel approaches
journal, February 2015


Disintegration of Meatball Electrodes for LiNi x Mn y Co z O2 Cathode Materials
journal, May 2017


Nano-structural changes in Li-ion battery cathodes during cycling revealed by FIB-SEM serial sectioning tomography
journal, January 2015

  • Song, Bohang; Sui, Tan; Ying, Siqi
  • Journal of Materials Chemistry A, Vol. 3, Issue 35
  • DOI: 10.1039/C5TA04151A

Intragranular cracking as a critical barrier for high-voltage usage of layer-structured cathode for lithium-ion batteries
journal, January 2017

  • Yan, Pengfei; Zheng, Jianming; Gu, Meng
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14101

Mesoscale Battery Science: The Behavior of Electrode Particles Caught on a Multispectral X-ray Camera
journal, June 2018


Three-dimensional imaging of chemical phase transformations at the nanoscale with full-field transmission X-ray microscopy
journal, July 2011

  • Meirer, Florian; Cabana, Jordi; Liu, Yijin
  • Journal of Synchrotron Radiation, Vol. 18, Issue 5
  • DOI: 10.1107/S0909049511019364

Mechanisms of Degradation and Strategies for the Stabilization of Cathode–Electrolyte Interfaces in Li-Ion Batteries
journal, January 2018


In situ X-ray diffraction studies of mixed LiMn2O4–LiNi1/3Co1/3Mn1/3O2 composite cathode in Li-ion cells during charge–discharge cycling
journal, July 2009


Persistent State-of-Charge Heterogeneity in Relaxed, Partially Charged Li 1− x Ni 1/3 Co 1/3 Mn 1/3 O 2 Secondary Particles
journal, May 2016

  • Gent, William E.; Li, Yiyang; Ahn, Sungjin
  • Advanced Materials, Vol. 28, Issue 31
  • DOI: 10.1002/adma.201601273

Charging Up Lithium-Ion Battery Cathodes
journal, March 2018


On the fragmentation of active material secondary particles in lithium ion battery cathodes induced by charge cycling
journal, December 2016


Multiscale Morphological and Electrical Characterization of Charge Transport Limitations to the Power Performance of Positive Electrode Blends for Lithium-Ion Batteries
journal, December 2016

  • Besnard, Nicolas; Etiemble, Aurélien; Douillard, Thierry
  • Advanced Energy Materials, Vol. 7, Issue 8
  • DOI: 10.1002/aenm.201602239

Profiling the nanoscale gradient in stoichiometric layered cathode particles for lithium-ion batteries
journal, January 2014

  • Lin, Feng; Nordlund, Dennis; Markus, Isaac M.
  • Energy & Environmental Science, Vol. 7, Issue 9
  • DOI: 10.1039/C4EE01400F

3D elemental sensitive imaging using transmission X-ray microscopy
journal, February 2012

  • Liu, Yijin; Meirer, Florian; Wang, Junyue
  • Analytical and Bioanalytical Chemistry, Vol. 404, Issue 5
  • DOI: 10.1007/s00216-012-5818-9

A new iterative algorithm to reconstruct the refractive index
journal, May 2007


TXM-Wizard : a program for advanced data collection and evaluation in full-field transmission X-ray microscopy
journal, January 2012

  • Liu, Yijin; Meirer, Florian; Williams, Phillip A.
  • Journal of Synchrotron Radiation, Vol. 19, Issue 2
  • DOI: 10.1107/S0909049511049144

    Works referencing / citing this record:

    Thermally driven mesoscale chemomechanical interplay in Li 0.5 Ni 0.6 Mn 0.2 Co 0.2 O 2 cathode materials
    journal, January 2018

    • Wei, Chenxi; Zhang, Yan; Lee, Sang-Jun
    • Journal of Materials Chemistry A, Vol. 6, Issue 45
    • DOI: 10.1039/c8ta08973f

    Quantification of Heterogeneous Degradation in Li‐Ion Batteries
    journal, May 2019


    Probing and quantifying cathode charge heterogeneity in Li ion batteries
    journal, January 2019

    • Zhang, Yuxin; Yang, Zhijie; Tian, Chixia
    • Journal of Materials Chemistry A, Vol. 7, Issue 41
    • DOI: 10.1039/c9ta06977a

    Chemomechanical behaviors of layered cathode materials in alkali metal ion batteries
    journal, January 2018

    • Xu, Zhengrui; Rahman, Muhammad Mominur; Mu, Linqin
    • Journal of Materials Chemistry A, Vol. 6, Issue 44
    • DOI: 10.1039/c8ta06875e

    Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials
    journal, January 2020


    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

    Automatic projection image registration for nanoscale X-ray tomographic reconstruction
    journal, October 2018


    Challenges and opportunities towards fast-charging battery materials
    journal, June 2019


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.