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Revealing causes of macroscale heterogeneity in lithium ion pouch cells via synchrotron X-ray diffraction

Journal Article · · Journal of Power Sources
Heterogeneous battery performance is a critical issue for maximization of cell lifetime capacity and safety. Using high energy synchrotron X-ray diffraction, the influence of charge rate, voltage limit, uneven stack pressure, and gas generation on the lithium transport properties was quantified in single-layer graphite/LiNi0.5Mn0.3Co0.2O2 pouch cells. A freshly formatted cell tracked in operando during initial fast charge cycles indicated variable position-dependent performances, while lateral mapping showed a significant fast charge (6C) heterogeneity compared to slow charge (C/2). Pressure effects were non-dominant compared to charge rate. Maps of previously aged and rested cells indicate that lateral heterogeneity slowly equilibrates at rest, but regenerates upon further cycling at fast charge rate. Furthermore, an unformatted cell was mapped at charge and discharge during its first formation cycle to analyze the effect of byproduct gases on the heterogeneous lithium transport. Gas was observed as randomly interspersed “bubbles” which locally hindered lithium intercalation and caused significant heterogeneity. Electrode architectures and charging protocols that promote homogeneous intercalation are critical for predictable high-performance and long-life batteries.
Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; AC07-05ID14517; AC36-08GO28308
OSTI ID:
1812322
Alternate ID(s):
OSTI ID: 1813290
OSTI ID: 1815123
OSTI ID: 1835291
Report Number(s):
INL/JOU--21-63347-Rev000; NREL/JA--5700-79879; MainId:39097; UUID:84e15974-0560-4117-aa43-16080969725a; MainAdminID:25774
Journal Information:
Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 507; ISSN 0378-7753
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (43)

Quantification of Heterogeneous Degradation in Li‐Ion Batteries journal May 2019
A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries journal October 2019
Using in operando diffraction to relate lattice strain with degradation mechanism in a NMC battery journal October 2018
Disintegration of Meatball Electrodes for LiNi x Mn y Co z O2 Cathode Materials journal May 2017
The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling journal August 2016
Electrode scale and electrolyte transport effects on extreme fast charging of lithium-ion cells journal March 2020
Nonlinear aging of cylindrical lithium-ion cells linked to heterogeneous compression journal February 2016
Lithium flow between active area and overhang of graphite anodes as a function of temperature and overhang geometry journal August 2019
Overcharging a lithium-ion battery: Effect on the LixC6 negative electrode determined by in situ neutron diffraction journal December 2013
Stress evolution and capacity fade in constrained lithium-ion pouch cells journal January 2014
Understanding structural changes in NMC Li-ion cells by in situ neutron diffraction journal June 2014
Enabling fast charging – A battery technology gap assessment journal November 2017
Effect of overcharge on Li(Ni0.5Mn0.3Co0.2)O2/graphite lithium ion cells with poly(vinylidene fluoride) binder. III — Chemical changes in the cathode journal May 2018
Effects of external pressure on the performance and ageing of single-layer lithium-ion pouch cells journal May 2018
Cost of automotive lithium-ion batteries operating at high upper cutoff voltages journal November 2018
Lithium heterogeneities in cylinder-type Li-ion batteries – fatigue induced by cycling journal February 2020
Heterogeneous Behavior of Lithium Plating during Extreme Fast Charging journal July 2020
XRD study of phase transformations in lithiated graphite anodes by Rietveld method journal May 2017
Synchrotron Operando Depth Profiling Studies of State-of-Charge Gradients in Thick Li(Ni 0.8 Mn 0.1 Co 0.1 )O 2 Cathode Films journal July 2020
Intercalation Compounds from LiH and Graphite: Relative Stability of Metastable Stages and Thermodynamic Stability of Dilute Stage I d journal March 2015
Reaction Heterogeneity in LiNi 0.8 Co 0.15 Al 0.05 O 2 Induced by Surface Layer journal August 2017
Thermodynamics of Antisite Defects in Layered NMC Cathodes: Systematic Insights from High-Precision Powder Diffraction Analyses journal December 2019
Kinetically Determined Phase Transition from Stage II (LiC 12 ) to Stage I (LiC 6 ) in a Graphite Anode for Li-Ion Batteries journal September 2018
Stability of Solid-Electrolyte Interphase (SEI) on the Lithium Metal Surface in Lithium Metal Batteries (LMBs) journal November 2020
In Situ Analysis of Gas Generation in Lithium-Ion Batteries with Different Carbonate-Based Electrolytes journal October 2015
Collapse of LiNi 1– xy Co x Mn y O 2 Lattice at Deep Charge Irrespective of Nickel Content in Lithium-Ion Batteries journal March 2019
Effects of Inhomogeneities—Nanoscale to Mesoscale—on the Durability of Li-Ion Batteries journal February 2013
Building ultraconformal protective layers on both secondary and primary particles of layered lithium transition metal oxide cathodes journal May 2019
Quantifying lithium concentration gradients in the graphite electrode of Li-ion cells using operando energy dispersive X-ray diffraction journal January 2019
Probing and quantifying cathode charge heterogeneity in Li ion batteries journal January 2019
Phase diagram of Li x C 6 journal November 1991
GSAS-II : the genesis of a modern open-source all purpose crystallography software package journal March 2013
Two-Dimensional Modeling of Lithium Deposition during Cell Charging journal January 2009
Oxygen Release and Its Effect on the Cycling Stability of LiNi x Mn y Co z O 2 (NMC) Cathode Materials for Li-Ion Batteries journal January 2017
Cycling Behavior of NCM523/Graphite Lithium-Ion Cells in the 3–4.4 V Range: Diagnostic Studies of Full Cells and Harvested Electrodes journal September 2016
Introduction to Electrochemical Impedance Spectroscopy as a Measurement Method for the Wetting Degree of Lithium-Ion Cells journal January 2018
A Volume Averaged Approach to the Numerical Modeling of Phase-Transition Intercalation Electrodes Presented for Li x C 6 journal January 2012
Lithium Intercalation into Graphitic Carbons Revisited: Experimental Evidence for Twisted Bilayer Behavior journal January 2013
Fast Charging of Li-Ion Cells: Part I. Using Li/Cu Reference Electrodes to Probe Individual Electrode Potentials journal January 2019
Operando X-ray Diffraction Study of Polycrystalline and Single-Crystal Li x Ni 0.5 Mn 0.3 Co 0.2 O 2 journal January 2017
Extreme Fast Charge Challenges for Lithium-Ion Battery: Variability and Positive Electrode Issues journal January 2019
The Effects of Defects on Localized Plating in Lithium-Ion Batteries journal January 2015
In Situ Neutron Diffraction Study of Lithiation Gradients in Graphite Anodes during Discharge and Relaxation journal January 2018