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

Xu, Rong; Yang, Yang; Yin, Fei; Liu, Pengfei; Cloetens, Peter; Liu, Yijin; Lin, Feng; Zhao, Kejie

doi:10.1016/j.jmps.2019.05.003

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

Journal Article · Sat May 11 00:00:00 EDT 2019 · Journal of the Mechanics and Physics of Solids

DOI:https://doi.org/10.1016/j.jmps.2019.05.003· OSTI ID:1546791

Xu, Rong ^[1]; Yang, Yang ^[2]; Yin, Fei ^[1]; Liu, Pengfei ^[1]; Cloetens, Peter ^[2]; Liu, Yijin ^[3]; Lin, Feng ^[4]; Zhao, Kejie ^[1]

Purdue Univ., West Lafayette, IN (United States)
European Synchrotron Radiation Facility, Grenoble (France)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)

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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF)

Grant/Contract Number:: CMMI-1726392; DMR-1832707; DMR-1832613; AC02-76SF00515

OSTI ID:: 1546791

Alternate ID(s):: OSTI ID: 1701809

Journal Information:: Journal of the Mechanics and Physics of Solids, Vol. 129, Issue C; ISSN 0022-5096

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 125 works

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