Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries
| dc.contributor.author | Liu, Pengfei | en |
| dc.contributor.author | Xu, Rong | en |
| dc.contributor.author | Liu, Yijin | en |
| dc.contributor.author | Lin, Feng | en |
| dc.contributor.author | Zhao, Kejie | en |
| dc.contributor.department | Chemistry | en |
| dc.date.accessioned | 2020-08-17T13:48:29Z | en |
| dc.date.available | 2020-08-17T13:48:29Z | en |
| dc.date.issued | 2020-03-05 | en |
| dc.description.abstract | 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 microstructureresolved 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. | en |
| dc.description.sponsorship | P. L. is grateful for the China Scholarship Council for a visiting scholarship at Purdue University. R. X. and K. Z. acknowledge the support by the National Science Foundation through the grants DMR-1832707 and CBET-1603866. F. L. acknowledges the support from the National Science Foundation under grant No. DMR-1832613. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. | en |
| dc.identifier.doi | https://doi.org/10.1149/1945-7111/ab78fa | en |
| dc.identifier.uri | http://hdl.handle.net/10919/99724 | en |
| dc.identifier.volume | 167 | en |
| dc.language.iso | en_US | en |
| dc.publisher | IOP Publishing Limited | en |
| dc.rights | Creative Commons Attribution 4.0 International | en |
| dc.rights.uri | http://creativecommons.org/licenses/by/4.0/ | en |
| dc.title | Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries | en |
| dc.title.serial | Journal of The Electrochemical Society | en |
| dc.type | Article - Refereed | en |