Journal
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
Volume 167, Issue 4, Pages -Publisher
ELECTROCHEMICAL SOC INC
DOI: 10.1149/1945-7111/ab78fa
Keywords
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Funding
- China Scholarship Council
- National Science Foundation [DMR-1832707, CBET-1603866, DMR-1832613]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
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Charge heterogeneity is a prevalent feature in many electrochemical systems. In a commercial cathode of Li-ion batteries, the composite is hierarchically structured across multiple length scales including the sub-micron single-crystal primary-particle domains up to the macroscopic particle ensembles. The redox kinetics of charge transfer and mass transport strongly couples with mechanical stresses. This interplay catalyzes substantial heterogeneity in the charge (re)distribution, stresses, and mechanical damage in the composite electrode during charging and discharging. We assess the heterogeneous electrochemistry and mechanics in a LiNixMnyCozO2 (NMC) cathode using a fully coupled electro-chemo-mechanics model at the cell level. A microstructure-resolved model is constructed based on the synchrotron X-ray tomography data. We calculate the stress field in the composite and then quantitatively evaluate the kinetics of surface charge transfer and Li transport biased by mechanical stresses. We further model the cyclic behavior of the cell. The repetitive deformation of the active particles and the weakening of the interfacial strength cause gradual increase of the interfacial debonding. The mechanical damage impedes electron transfer, incurs more charge heterogeneity, and results in the capacity degradation in batteries over cycles. (c) 2020 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited.
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