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

Title: Disintegration of Meatball Electrodes for LiNi x Mn y Co z O2 Cathode Materials

Journal Article · · Experimental Mechanics
 [1];  [1];  [1];  [2];  [1]
  1. Purdue Univ., West Lafayette, IN (United States). School of Mechanical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division

Mechanical degradation of Li-ion batteries caused by the repetitive swelling and shrinking of electrodes upon electrochemical cycles is now well recognized. Structural disintegration of the state-of-art cathode materials of a hierarchical structure is relatively less studied. We track the microstructural evolution of different marked regimes in LiNi x Mn y Co z O2 (NMC) electrodes after lithiation cycles. Decohesion of primary particles constitutes the major mechanical degradation in the NMC materials, which results in the loss of connectivity of the conductive network and impedance increase. We find that the structural disintegration is largely dependent on the charging rate – slow charging causes more damage, and is relatively insensitive to the cyclic voltage window. We use finite element modeling to study the evolution of Li concentration and stresses in a NMC secondary particle and employ the cohesive zone model to simulate the interfacial fracture between primary particles. We reveal that microcracks accumulate and propagate during the cyclic lithiation and delithiation at a slow charging rate.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Purdue Univ., West Lafayette, IN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF); Office of Naval Research (ONR) (United States); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
AC05-00OR22725; CBET-1603866
OSTI ID:
1424455
Alternate ID(s):
OSTI ID: 1474506
Journal Information:
Experimental Mechanics, Vol. 58, Issue 4; ISSN 0014-4851
Publisher:
SpringerCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 65 works
Citation information provided by
Web of Science

References (40)

The mechanics of large-volume-change transformations in high-capacity battery materials journal December 2016
Kinetics and fracture resistance of lithiated silicon nanostructure pairs controlled by their mechanical interaction journal June 2015
Grid indentation analysis of mechanical properties of composite electrodes in Li-ion batteries journal December 2016
Investigation of Structural Fatigue in Spinel Electrodes Using In Situ Laser Probe Beam Deflection Technique journal January 2002
Issues and challenges facing rechargeable lithium batteries journal November 2001
Effect of periodic surface cracks on the interfacial fracture of thermal barrier coating system journal October 2012
Cathode materials review
  • Daniel, Claus; Mohanty, Debasish; Li, Jianlin
  • REVIEW ON ELECTROCHEMICAL STORAGE MATERIALS AND TECHNOLOGY: Proceedings of the 1st International Freiberg Conference on Electrochemical Storage Materials, AIP Conference Proceedings https://doi.org/10.1063/1.4878478
conference January 2014
Materials processing for lithium-ion batteries journal March 2011
Mechanical interactions regulated kinetics and morphology of composite electrodes in Li-ion batteries journal September 2016
Understanding the role of mechanics in energy materials: A perspective journal December 2016
Evaluation Residual Moisture in Lithium-Ion Battery Electrodes and Its Effect on Electrode Performance journal January 2016
Structural transformation of a lithium-rich Li1.2Co0.1Mn0.55Ni0.15O2 cathode during high voltage cycling resolved by in situ X-ray diffraction journal May 2013
Kinetics Tuning of Li-Ion Diffusion in Layered Li(Ni x Mn y Co z )O 2 journal June 2015
Structural evolution and the capacity fade mechanism upon long-term cycling in Li-rich cathode material journal January 2012
Reversible Nanopore Formation in Ge Nanowires during Lithiation–Delithiation Cycling: An In Situ Transmission Electron Microscopy Study journal September 2011
Design criteria for electrochemical shock resistant battery electrodes journal January 2012
High-Voltage Performance of Li[Ni[sub 0.55]Co[sub 0.15]Mn[sub 0.30]]O[sub 2] Positive Electrode Material for Rechargeable Li-Ion Batteries journal January 2011
EIS study on the formation of solid electrolyte interface in Li-ion battery journal January 2006
Observation of Microstructural Evolution in Li Battery Cathode Oxide Particles by In Situ Electron Microscopy journal May 2013
A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries journal September 2010
Stepwise Nanopore Evolution in One-Dimensional Nanostructures journal April 2010
Stress Evolution in Lithium-Ion Composite Electrodes during Electrochemical Cycling and Resulting Internal Pressures on the Cell Casing journal January 2015
Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation journal August 2011
Computational analysis of chemomechanical behaviors of composite electrodes in Li-ion batteries journal August 2016
Oxygen Vacancies Lead to Loss of Domain Order, Particle Fracture, and Rapid Capacity Fade in Lithium Manganospinel (LiMn 2 O 4 ) Batteries journal May 2014
Reactive Flow in Silicon Electrodes Assisted by the Insertion of Lithium journal July 2012
Capacity fading of LiAlyNi1−x−yCoxO2 cathode for lithium-ion batteries during accelerated calendar and cycle life tests (effect of depth of discharge in charge–discharge cycling on the suppression of the micro-crack generation of LiAlyNi1−x−yCoxO2 particle) journal August 2014
On the fragmentation of active material secondary particles in lithium ion battery cathodes induced by charge cycling journal December 2016
Size-Dependent Fracture of Silicon Nanoparticles During Lithiation journal January 2012
Understanding the accumulated cycle capacity fade caused by the secondary particle fracture of LiNi1-x-yCoxMnyO2 cathode for lithium ion batteries journal October 2016
Interfacial Properties of the a-Si∕Cu:Active–Inactive Thin-Film Anode System for Lithium-Ion Batteries journal January 2006
Materials Challenges Facing Electrical Energy Storage journal April 2008
A pomegranate-inspired nanoscale design for large-volume-change lithium battery anodes journal February 2014
Lithium-Assisted Plastic Deformation of Silicon Electrodes in Lithium-Ion Batteries: A First-Principles Theoretical Study journal July 2011
Chemomechanical modeling of lithiation-induced failure in high-volume-change electrode materials for lithium ion batteries journal February 2017
TEM Study of Electrochemical Cycling-Induced Damage and Disorder in LiCoO[sub 2] Cathodes for Rechargeable Lithium Batteries journal January 1999
Study of the Failure Mechanisms of LiNi 0.8 Mn 0.1 Co 0.1 O 2 Cathode Material for Lithium Ion Batteries journal January 2015
In Situ Stress Evolution in Li 1+x Mn 2 O 4 Thin Films during Electrochemical Cycling in Li-Ion Cells journal January 2016
Crystal and electronic structures of superstructural Li1−x[Co1/3Ni1/3Mn1/3]O2 (0≤x≤1) journal June 2003
High-rate lithiation-induced reactivation of mesoporous hollow spheres for long-lived lithium-ion batteries journal July 2014

Cited By (9)

High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material journal March 2019
Dopant Segregation Boosting High‐Voltage Cyclability of Layered Cathode for Sodium Ion Batteries journal September 2019
Quantification of Heterogeneous Degradation in Li‐Ion Batteries journal May 2019
Effects of Charge Cutoff Potential on an Electrolyte Additive for LiNi 0.6 Co 0.2 Mn 0.2 O 2 –Mesocarbon Microbead Full Cells journal March 2019
Mechanistic understanding of intergranular cracking in NCM cathode material: mesoscale simulation with three-dimensional microstructure journal January 2018
Nickel enrichment of next-generation NMC nanomaterials alters material stability, causing unexpected dissolution behavior and observed toxicity to S. oneidensis MR-1 and D. magna journal January 2020
The Influence of Surface Stress on the Chemo-Mechanical Behavior of Inverse-Opal-Structured Electrodes for Lithium-Ion Batteries journal January 2020
Communication—Fracture Behavior of Single LiNi 0.33 Mn 0.33 Co 0.33 O 2 Particles Studied by Flat Punch Indentation journal January 2019
Challenges of Fast Charging for Electric Vehicles and the Role of Red Phosphorous as Anode Material: Review journal October 2019