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Title: Grid indentation analysis of mechanical properties of composite electrodes in Li-ion batteries

Journal Article · · Extreme Mechanics Letters
ORCiD logo [1];  [1]; ORCiD logo [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

We report that electrodes in commercial rechargeable batteries are microscopically heterogeneous materials. The constituent components, including active materials, polymeric binders, and porous conductive matrix, often have large variation in their mechanical properties, making the mechanical characterization of composite electrodes a challenging task. In a model system of LiNi0.5Mn0.3Co0.2O2 cathode, we employ the instrumented grid indentation to determine the elastic modulus and hardness of the constituent phases. The approach relies on a large array of nanoindentation experiments and statistical analysis of the resulting data provided that the maximum indentation depth is carefully chosen. The statistically extracted properties of the active particles and the surrounding medium are in good agreement with the tests of targeted indentation at selected sites. Lastly, the combinatory technique of grid indentation and statistical deconvolution represents a fast and reliable route to quantify the mechanical properties of composite electrodes that feed the parametric input for the mechanics models.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1302942
Alternate ID(s):
OSTI ID: 1397349
Journal Information:
Extreme Mechanics Letters, Journal Name: Extreme Mechanics Letters; ISSN 2352-4316
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 65 works
Citation information provided by
Web of Science

References (40)

Building better batteries journal February 2008
Materials Challenges Facing Electrical Energy Storage journal April 2008
Issues and challenges facing rechargeable lithium batteries journal November 2001
Deformation and stress in electrode materials for Li-ion batteries journal June 2014
Alloy Negative Electrodes for Li-Ion Batteries journal October 2014
Capacity fade study of lithium-ion batteries cycled at high discharge rates journal May 2003
Elastic Properties of the Solid Electrolyte Li 7 La 3 Zr 2 O 12 (LLZO) journal December 2015
Development of Electrolytes towards Achieving Safe and High-Performance Energy-Storage Devices: A Review journal September 2014
Stress generation and fracture in lithium insertion materials journal March 2006
Diffusion-Induced Stress, Interfacial Charge Transfer, and Criteria for Avoiding Crack Initiation of Electrode Particles journal January 2010
Method to deduce the critical size for interfacial delamination of patterned electrode structures and application to lithiation of thin-film silicon islands journal May 2012
A finite strain model of stress, diffusion, plastic flow, and electrochemical reactions in a lithium-ion half-cell journal April 2011
A finite deformation stress-dependent chemical potential and its applications to lithium ion batteries journal July 2012
Large Plastic Deformation in High-Capacity Lithium-Ion Batteries Caused by Charge and Discharge: Large Plastic Deformation in Lithium-Ion Batteries journal March 2011
A chemo-mechanical model of lithiation in silicon journal October 2014
Lithiation induced corrosive fracture in defective carbon nanotubes journal October 2013
Lithiation of SiO 2 in Li-Ion Batteries: In Situ Transmission Electron Microscopy Experiments and Theoretical Studies journal November 2014
Cyclic plasticity and shakedown in high-capacity electrodes of lithium-ion batteries journal April 2013
Concurrent Reaction and Plasticity during Initial Lithiation of Crystalline Silicon in Lithium-Ion Batteries journal January 2012
Kinetics of Initial Lithiation of Crystalline Silicon Electrodes of Lithium-Ion Batteries journal January 2012
Fracture Toughness Characterization of Lithiated Germanium as an Anode Material for Lithium-Ion Batteries journal November 2015
In situ measurements of stress evolution in silicon thin films during electrochemical lithiation and delithiation journal August 2010
Stress Evolution in Lithium-Ion Composite Electrodes during Electrochemical Cycling and Resulting Internal Pressures on the Cell Casing journal January 2015
Strong kinetics-stress coupling in lithiation of Si and Ge anodes journal March 2015
Modeling Crack Growth during Li Extraction in Storage Particles Using a Fracture Phase Field Approach journal November 2015
Electrochemically driven mechanical energy harvesting journal January 2016
Fracture of electrodes in lithium-ion batteries caused by fast charging journal October 2010
An Analytical Method to Determine Tortuosity in Rechargeable Battery Electrodes journal January 2012
Threefold Increase in the Young’s Modulus of Graphite Negative Electrode during Lithium Intercalation journal January 2010
Lithium-Assisted Plastic Deformation of Silicon Electrodes in Lithium-Ion Batteries: A First-Principles Theoretical Study journal July 2011
Brittle-to-ductile transition of lithiated silicon electrodes: Crazing to stable nanopore growth journal September 2015
Brittle versus ductile fracture mechanism transition in amorphous lithiated silicon: From intrinsic nanoscale cavitation to shear banding journal November 2015
Grid indentation analysis of composite microstructure and mechanics: Principles and validation journal August 2006
Statistical Indentation Techniques for Hydrated Nanocomposites: Concrete, Bone, and Shale journal September 2007
Layered Lithium Insertion Material of LiNi 1/2 Mn 1/2 O 2 : A Possible Alternative to LiCoO 2 for Advanced Lithium-Ion Batteries journal August 2001
Layered Li[Ni[sub x]Co[sub 1−2x]Mn[sub x]]O[sub 2] Cathode Materials for Lithium-Ion Batteries journal January 2001
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
Understanding the structure and structural degradation mechanisms in high-voltage, lithium-manganese–rich lithium-ion battery cathode oxides: A review of materials diagnostics journal January 2015
Comparison of Isolated Indentation and Grid Indentation Methods for HVOF Sprayed Cermets journal January 2012
An improved technique for determining hardness and elastic modulus using load and displacement sensing indentation experiments journal June 1992

Cited By (8)

Operando Nanoindentation: A New Platform to Measure the Mechanical Properties of Electrodes during Electrochemical Reactions journal January 2017
Mechanical characterization by multiscale instrumented indentation of highly heterogeneous materials for braking applications journal November 2018
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
Failure modes and mechanisms for rechargeable Lithium-based batteries: a state-of-the-art review journal November 2018
Chemomechanical modeling of lithiation-induced failure in high-volume-change electrode materials for lithium ion batteries journal February 2017
Three‐dimensional simulation of transport processes within blended electrodes on the particle scale journal July 2019
Mechanistic understanding of intergranular cracking in NCM cathode material: mesoscale simulation with three-dimensional microstructure journal January 2018
Three‐dimensional simulation of transport processes within blended electrodes on the particle scale text January 2019