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Title: Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling

Abstract

We assess the heterogeneous electrochemistry and mechanics in a composite electrode of commercial batteries using synchrotron X-ray tomography analysis and microstructure-resolved computational modeling. We visualize the morphological defects at multi-scales ranging from the macroscopic composite, particle ensembles, to individual single particles. Particle fracture and interfacial debonding are identified in a large set of tomographic data of active particles. Mechanical failure in the regime near the separator is more severe than toward the current collector. The active particles close to the separator experience deeper charge and discharge over cycles and thus are more mechanically loaded. The difference in the Li activity originates from the polarization of the electrolyte potential and the non-uniform distribution of the activation energy for the charge transfer reaction. We model the kinetics of intergranular fracture and interfacial degradation to confirm that the various Li activities are the major cause of the heterogeneous damage. The interfacial failure may reconstruct the conductive network and redistribute the electrochemical activities that render a dynamic nature of electrochemistry and mechanics evolving over time in the composite electrode. We further quantify the influence of the mechanical damage on the metrics of battery performance. We simulate the electrochemical impedance profile to build a relationshipmore » between the interfacial debonding and the impedance of electron transport and surface charge transfer. Lastly, the mechanical failure disrupts the conduction path of electrons and results in significant polarization and capacity loss in batteries.« less

Authors:
 [1];  [2];  [1];  [1];  [2];  [3];  [4];  [1]
  1. Purdue Univ., West Lafayette, IN (United States)
  2. European Synchrotron Radiation Facility, Grenoble (France)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  4. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE; National Science Foundation (NSF)
OSTI Identifier:
1546791
Alternate Identifier(s):
OSTI ID: 1701809
Grant/Contract Number:  
CMMI-1726392; DMR-1832707; DMR-1832613; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Mechanics and Physics of Solids
Additional Journal Information:
Journal Volume: 129; Journal Issue: C; Journal ID: ISSN 0022-5096
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Heterogeneous degradation; Fracture; Interfacial debonding; NMC; Batteries

Citation Formats

Xu, Rong, Yang, Yang, Yin, Fei, Liu, Pengfei, Cloetens, Peter, Liu, Yijin, Lin, Feng, and Zhao, Kejie. Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling. United States: N. p., 2019. Web. https://doi.org/10.1016/j.jmps.2019.05.003.
Xu, Rong, Yang, Yang, Yin, Fei, Liu, Pengfei, Cloetens, Peter, Liu, Yijin, Lin, Feng, & Zhao, Kejie. Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling. United States. https://doi.org/10.1016/j.jmps.2019.05.003
Xu, Rong, Yang, Yang, Yin, Fei, Liu, Pengfei, Cloetens, Peter, Liu, Yijin, Lin, Feng, and Zhao, Kejie. Sat . "Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling". United States. https://doi.org/10.1016/j.jmps.2019.05.003. https://www.osti.gov/servlets/purl/1546791.
@article{osti_1546791,
title = {Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling},
author = {Xu, Rong and Yang, Yang and Yin, Fei and Liu, Pengfei and Cloetens, Peter and Liu, Yijin and Lin, Feng and Zhao, Kejie},
abstractNote = {We assess the heterogeneous electrochemistry and mechanics in a composite electrode of commercial batteries using synchrotron X-ray tomography analysis and microstructure-resolved computational modeling. We visualize the morphological defects at multi-scales ranging from the macroscopic composite, particle ensembles, to individual single particles. Particle fracture and interfacial debonding are identified in a large set of tomographic data of active particles. Mechanical failure in the regime near the separator is more severe than toward the current collector. The active particles close to the separator experience deeper charge and discharge over cycles and thus are more mechanically loaded. The difference in the Li activity originates from the polarization of the electrolyte potential and the non-uniform distribution of the activation energy for the charge transfer reaction. We model the kinetics of intergranular fracture and interfacial degradation to confirm that the various Li activities are the major cause of the heterogeneous damage. The interfacial failure may reconstruct the conductive network and redistribute the electrochemical activities that render a dynamic nature of electrochemistry and mechanics evolving over time in the composite electrode. We further quantify the influence of the mechanical damage on the metrics of battery performance. We simulate the electrochemical impedance profile to build a relationship between the interfacial debonding and the impedance of electron transport and surface charge transfer. Lastly, the mechanical failure disrupts the conduction path of electrons and results in significant polarization and capacity loss in batteries.},
doi = {10.1016/j.jmps.2019.05.003},
journal = {Journal of the Mechanics and Physics of Solids},
number = C,
volume = 129,
place = {United States},
year = {2019},
month = {5}
}

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Cited by: 14 works
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