skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode

Abstract

Electrochemically driven functioning of a battery inevitably induces thermal and mechanical effects, which in turn couple with the electrochemical effect and collectively govern the performance of the battery. However, such a coupling effect, whether favorable or detrimental, has never been explicitly elucidated. Here we use in situ transmission electron microscopy to demonstrate such a coupling effect. We discover that thermally perturbating delithiated LiNi 0.6Mn 0.2Co 0.2O 2 will trigger explosive nucleation and propagation of intragranular cracks in the lattice, providing us a unique opportunity to directly visualize the cracking mechanism and dynamics. We reveal that thermal stress associated with electrochemically induced phase inhomogeneity and internal pressure resulting from oxygen release are the primary driving forces for intragranular cracking that resembles a “popcorn” fracture mechanism. The present work reveals that, for battery performance, the intricate coupling of electrochemical, thermal, and mechanical effects will surpass the superposition of individual effects.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4];  [5];  [5]; ORCiD logo [5]; ORCiD logo [2];  [3]; ORCiD logo [4]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab.; Beijing Univ. of Technology (China). Inst. of Microstructure and Properties of Advanced Materials
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
  3. Pennsylvania State Univ., University Park, PA (United States). Dept. of Engineering Science and Mechanics
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab.
  5. Beijing Univ. of Technology (China). Inst. of Microstructure and Properties of Advanced Materials
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Pennsylvania State Univ., University Park, PA (United States); Beijing Univ. of Technology (China)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Science Foundation (NSF); Chinese National Natural Science Fund for Innovative Research Groups; National Key Research and Development Program of China
OSTI Identifier:
1514257
Report Number(s):
PNNL-SA-134810
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC05-76RL01830; AC02-05CH11231; CMMI-0900692; DMR-1610430; ECCS-1610331; 51621003; 2016YFB0700700
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; batteries

Citation Formats

Yan, Pengfei, Zheng, Jianming, Chen, Tianwu, Luo, Langli, Jiang, Yuyuan, Wang, Kuan, Sui, Manling, Zhang, Ji-Guang, Zhang, Sulin, and Wang, Chongmin. Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04862-w.
Yan, Pengfei, Zheng, Jianming, Chen, Tianwu, Luo, Langli, Jiang, Yuyuan, Wang, Kuan, Sui, Manling, Zhang, Ji-Guang, Zhang, Sulin, & Wang, Chongmin. Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode. United States. doi:10.1038/s41467-018-04862-w.
Yan, Pengfei, Zheng, Jianming, Chen, Tianwu, Luo, Langli, Jiang, Yuyuan, Wang, Kuan, Sui, Manling, Zhang, Ji-Guang, Zhang, Sulin, and Wang, Chongmin. Fri . "Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode". United States. doi:10.1038/s41467-018-04862-w. https://www.osti.gov/servlets/purl/1514257.
@article{osti_1514257,
title = {Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode},
author = {Yan, Pengfei and Zheng, Jianming and Chen, Tianwu and Luo, Langli and Jiang, Yuyuan and Wang, Kuan and Sui, Manling and Zhang, Ji-Guang and Zhang, Sulin and Wang, Chongmin},
abstractNote = {Electrochemically driven functioning of a battery inevitably induces thermal and mechanical effects, which in turn couple with the electrochemical effect and collectively govern the performance of the battery. However, such a coupling effect, whether favorable or detrimental, has never been explicitly elucidated. Here we use in situ transmission electron microscopy to demonstrate such a coupling effect. We discover that thermally perturbating delithiated LiNi0.6Mn0.2Co0.2O2 will trigger explosive nucleation and propagation of intragranular cracks in the lattice, providing us a unique opportunity to directly visualize the cracking mechanism and dynamics. We reveal that thermal stress associated with electrochemically induced phase inhomogeneity and internal pressure resulting from oxygen release are the primary driving forces for intragranular cracking that resembles a “popcorn” fracture mechanism. The present work reveals that, for battery performance, the intricate coupling of electrochemical, thermal, and mechanical effects will surpass the superposition of individual effects.},
doi = {10.1038/s41467-018-04862-w},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 33 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Cycling performance and cracks of LiNi0.6Mn0.2Co0.2O2. a Capacity decay and b corresponding charge–discharge voltage profile evolution at cycling window 2.7–4.8 V. Cross-sectional high angle dark field (HAADF) images from (c) pristine sample d, e after 100 cycles at 2.7–4.5 V, f–h after 100 cycles at 2.7–4.8 V. Redmore » arrow in (d) highlights intergranular cracks formed during cycling. Red arrows in (f, g) highlight some intragranular cracks within primary particles. Yellow arrows in (g, h) highlight incubation cracks. The scale bars are 500 nm in (c–f), 10 nm in (g) and 2 nm in (h)« less

Save / Share:

Works referenced in this record:

Recent advances in the Si-based nanocomposite materials as high capacity anode materials for lithium ion batteries
journal, July 2014


X-ray/Neutron Diffraction and Electrochemical Studies of Lithium De/Re-Intercalation in Li 1 - x Co 1/ 3 Ni 1/3 Mn 1/3 O 2 ( x = 0 → 1)
journal, April 2006

  • Yin, S. -C.; Rho, Y. -H.; Swainson, I.
  • Chemistry of Materials, Vol. 18, Issue 7
  • DOI: 10.1021/cm0511769

Tuning the Activity of Oxygen in LiNi 0.8 Co 0.15 Al 0.05 O 2 Battery Electrodes
journal, October 2016

  • Karki, Khim; Huang, Yiqing; Hwang, Sooyeon
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 41
  • DOI: 10.1021/acsami.6b09585

Thermal Instability of Cycled Li x Ni 0.5 Mn 0.5 O 2 Electrodes: An in Situ Synchrotron X-ray Powder Diffraction Study
journal, August 2008

  • Yabuuchi, Naoaki; Kim, Yong-Tae; Li, Hayley H.
  • Chemistry of Materials, Vol. 20, Issue 15
  • DOI: 10.1021/cm800314d

Cobalt dissolution in LiCoO2-based non-aqueous rechargeable batteries
journal, January 1996


Deformation and stress in electrode materials for Li-ion batteries
journal, June 2014


Electrolytes and Interphases in Li-Ion Batteries and Beyond
journal, October 2014


High-voltage positive electrode materials for lithium-ion batteries
journal, January 2017

  • Li, Wangda; Song, Bohang; Manthiram, Arumugam
  • Chemical Society Reviews, Vol. 46, Issue 10
  • DOI: 10.1039/C6CS00875E

Surface-Coating Regulated Lithiation Kinetics and Degradation in Silicon Nanowires for Lithium Ion Battery
journal, April 2015


Enhanced Li+ ion transport in LiNi0.5Mn1.5O4 through control of site disorder
journal, January 2012

  • Zheng, Jianming; Xiao, Jie; Yu, Xiqian
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 39
  • DOI: 10.1039/c2cp43007j

Nanostructured high-energy cathode materials for advanced lithium batteries
journal, October 2012

  • Sun, Yang-Kook; Chen, Zonghai; Noh, Hyung-Joo
  • Nature Materials, Vol. 11, Issue 11
  • DOI: 10.1038/nmat3435

Anisotropic Lattice Strain and Mechanical Degradation of High- and Low-Nickel NCM Cathode Materials for Li-Ion Batteries
journal, February 2017

  • Kondrakov, Aleksandr O.; Schmidt, Alexander; Xu, Jin
  • The Journal of Physical Chemistry C, Vol. 121, Issue 6
  • DOI: 10.1021/acs.jpcc.6b12885

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


Phosphorus Enrichment as a New Composition in the Solid Electrolyte Interphase of High-Voltage Cathodes and Its Effects on Battery Cycling
journal, October 2015


Development of Microstrain in Aged Lithium Transition Metal Oxides
journal, June 2014

  • Lee, Eung-Ju; Chen, Zonghai; Noh, Hyung-Ju
  • Nano Letters, Vol. 14, Issue 8
  • DOI: 10.1021/nl5022859

Review—Li-Rich Layered Oxide Cathodes for Next-Generation Li-Ion Batteries: Chances and Challenges
journal, January 2015

  • Rozier, Patrick; Tarascon, Jean Marie
  • Journal of The Electrochemical Society, Vol. 162, Issue 14
  • DOI: 10.1149/2.0111514jes

Review—High-Capacity Li[Ni 1- x Co x /2 Mn x /2 ]O 2 ( x = 0.1, 0.05, 0) Cathodes for Next-Generation Li-Ion Battery
journal, January 2015

  • Yoon, Chong S.; Choi, Moon Ho; Lim, Byung-Beom
  • Journal of The Electrochemical Society, Vol. 162, Issue 14
  • DOI: 10.1149/2.0101514jes

Uncovering the roles of oxygen vacancies in cation migration in lithium excess layered oxides
journal, January 2014

  • Qian, Danna; Xu, Bo; Chi, Miaofang
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 28
  • DOI: 10.1039/C4CP01799D

Reviving the lithium metal anode for high-energy batteries
journal, March 2017

  • Lin, Dingchang; Liu, Yayuan; Cui, Yi
  • Nature Nanotechnology, Vol. 12, Issue 3
  • DOI: 10.1038/nnano.2017.16

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


The role of nanotechnology in the development of battery materials for electric vehicles
journal, December 2016


Facet-Dependent Thermal Instability in LiCoO 2
journal, March 2017


Nickel-Rich and Lithium-Rich Layered Oxide Cathodes: Progress and Perspectives
journal, October 2015

  • Manthiram, Arumugam; Knight, James C.; Myung, Seung-Taek
  • Advanced Energy Materials, Vol. 6, Issue 1
  • DOI: 10.1002/aenm.201501010

Correlating Structural Changes and Gas Evolution during the Thermal Decomposition of Charged Li x Ni 0.8 Co 0.15 Al 0.05 O 2 Cathode Materials
journal, January 2013

  • Bak, Seong-Min; Nam, Kyung-Wan; Chang, Wonyoung
  • Chemistry of Materials, Vol. 25, Issue 3
  • DOI: 10.1021/cm303096e

Structural Changes and Thermal Stability of Charged LiNi x Mn y Co z O 2 Cathode Materials Studied by Combined In Situ Time-Resolved XRD and Mass Spectroscopy
journal, December 2014

  • Bak, Seong-Min; Hu, Enyuan; Zhou, Yongning
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 24
  • DOI: 10.1021/am506712c

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

Intrinsic Origins of Crack Generation in Ni-rich LiNi0.8Co0.1Mn0.1O2 Layered Oxide Cathode Material
journal, January 2017

  • Lim, Jin-Myoung; Hwang, Taesoon; Kim, Duho
  • Scientific Reports, Vol. 7, Issue 1
  • DOI: 10.1038/srep39669

    Works referencing / citing this record:

    Enhanced Li+ ion transport in LiNi0.5Mn1.5O4 through control of site disorder
    journal, January 2012

    • Zheng, Jianming; Xiao, Jie; Yu, Xiqian
    • Physical Chemistry Chemical Physics, Vol. 14, Issue 39
    • DOI: 10.1039/c2cp43007j

    Facet-Dependent Thermal Instability in LiCoO 2
    journal, March 2017


    Deformation and stress in electrode materials for Li-ion batteries
    journal, June 2014


    Correlating Structural Changes and Gas Evolution during the Thermal Decomposition of Charged Li x Ni 0.8 Co 0.15 Al 0.05 O 2 Cathode Materials
    journal, January 2013

    • Bak, Seong-Min; Nam, Kyung-Wan; Chang, Wonyoung
    • Chemistry of Materials, Vol. 25, Issue 3
    • DOI: 10.1021/cm303096e

    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

    Cobalt dissolution in LiCoO2-based non-aqueous rechargeable batteries
    journal, January 1996


    Review—High-Capacity Li[Ni 1- x Co x /2 Mn x /2 ]O 2 ( x = 0.1, 0.05, 0) Cathodes for Next-Generation Li-Ion Battery
    journal, January 2015

    • Yoon, Chong S.; Choi, Moon Ho; Lim, Byung-Beom
    • Journal of The Electrochemical Society, Vol. 162, Issue 14
    • DOI: 10.1149/2.0101514jes

    Nanostructured high-energy cathode materials for advanced lithium batteries
    journal, October 2012

    • Sun, Yang-Kook; Chen, Zonghai; Noh, Hyung-Joo
    • Nature Materials, Vol. 11, Issue 11
    • DOI: 10.1038/nmat3435

    Development of Microstrain in Aged Lithium Transition Metal Oxides
    journal, June 2014

    • Lee, Eung-Ju; Chen, Zonghai; Noh, Hyung-Ju
    • Nano Letters, Vol. 14, Issue 8
    • DOI: 10.1021/nl5022859

    The role of nanotechnology in the development of battery materials for electric vehicles
    journal, December 2016


    Tuning the Activity of Oxygen in LiNi 0.8 Co 0.15 Al 0.05 O 2 Battery Electrodes
    journal, October 2016

    • Karki, Khim; Huang, Yiqing; Hwang, Sooyeon
    • ACS Applied Materials & Interfaces, Vol. 8, Issue 41
    • DOI: 10.1021/acsami.6b09585

    Phosphorus Enrichment as a New Composition in the Solid Electrolyte Interphase of High-Voltage Cathodes and Its Effects on Battery Cycling
    journal, October 2015


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


    Nickel-Rich and Lithium-Rich Layered Oxide Cathodes: Progress and Perspectives
    journal, October 2015

    • Manthiram, Arumugam; Knight, James C.; Myung, Seung-Taek
    • Advanced Energy Materials, Vol. 6, Issue 1
    • DOI: 10.1002/aenm.201501010

    Thermal Instability of Cycled Li x Ni 0.5 Mn 0.5 O 2 Electrodes: An in Situ Synchrotron X-ray Powder Diffraction Study
    journal, August 2008

    • Yabuuchi, Naoaki; Kim, Yong-Tae; Li, Hayley H.
    • Chemistry of Materials, Vol. 20, Issue 15
    • DOI: 10.1021/cm800314d

    Electrolytes and Interphases in Li-Ion Batteries and Beyond
    journal, October 2014


    Structural Changes and Thermal Stability of Charged LiNi x Mn y Co z O 2 Cathode Materials Studied by Combined In Situ Time-Resolved XRD and Mass Spectroscopy
    journal, December 2014

    • Bak, Seong-Min; Hu, Enyuan; Zhou, Yongning
    • ACS Applied Materials & Interfaces, Vol. 6, Issue 24
    • DOI: 10.1021/am506712c

    Surface-Coating Regulated Lithiation Kinetics and Degradation in Silicon Nanowires for Lithium Ion Battery
    journal, April 2015


    X-ray/Neutron Diffraction and Electrochemical Studies of Lithium De/Re-Intercalation in Li 1 - x Co 1/ 3 Ni 1/3 Mn 1/3 O 2 ( x = 0 → 1)
    journal, April 2006

    • Yin, S. -C.; Rho, Y. -H.; Swainson, I.
    • Chemistry of Materials, Vol. 18, Issue 7
    • DOI: 10.1021/cm0511769

    Intrinsic Origins of Crack Generation in Ni-rich LiNi0.8Co0.1Mn0.1O2 Layered Oxide Cathode Material
    journal, January 2017

    • Lim, Jin-Myoung; Hwang, Taesoon; Kim, Duho
    • Scientific Reports, Vol. 7, Issue 1
    • DOI: 10.1038/srep39669

    Review—Li-Rich Layered Oxide Cathodes for Next-Generation Li-Ion Batteries: Chances and Challenges
    journal, January 2015

    • Rozier, Patrick; Tarascon, Jean Marie
    • Journal of The Electrochemical Society, Vol. 162, Issue 14
    • DOI: 10.1149/2.0111514jes

    Reviving the lithium metal anode for high-energy batteries
    journal, March 2017

    • Lin, Dingchang; Liu, Yayuan; Cui, Yi
    • Nature Nanotechnology, Vol. 12, Issue 3
    • DOI: 10.1038/nnano.2017.16

    Recent advances in the Si-based nanocomposite materials as high capacity anode materials for lithium ion batteries
    journal, July 2014


    Anisotropic Lattice Strain and Mechanical Degradation of High- and Low-Nickel NCM Cathode Materials for Li-Ion Batteries
    journal, February 2017

    • Kondrakov, Aleksandr O.; Schmidt, Alexander; Xu, Jin
    • The Journal of Physical Chemistry C, Vol. 121, Issue 6
    • DOI: 10.1021/acs.jpcc.6b12885

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


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