An atomistically informed mesoscale model for growth and coarsening during discharge in lithium-oxygen batteries

Welland, Michael J.; Lau, Kah Chun; Redfern, Paul C.; Liang, Linyun; Zhai, Denyun; Wolf, Dieter; Curtiss, Larry A.

doi:10.1063/1.4936410

Title: An atomistically informed mesoscale model for growth and coarsening during discharge in lithium-oxygen batteries

Journal Article · Thu Dec 10 00:00:00 EST 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4936410· OSTI ID:1287335

^[1]; Lau, Kah Chun ^[1];

^[1]; Liang, Linyun ^[2]; Zhai, Denyun ^[3]; Wolf, Dieter ^[1]; Curtiss, Larry A. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Argonne National Lab. (ANL), Argonne, IL (United States). Mathematics and Computer Science
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division

An atomistically informed mesoscale model is developed for the deposition of a discharge product in a Li-O₂ battery. This mescocale model includes particle growth and coarsening as well as a simplified nucleation model. The model involves LiO₂ formation through reaction of O₂^- and Li⁺ in the electrolyte, which deposits on the cathode surface when the LiO₂ concentration reaches supersaturation in the electrolyte. A reaction-diffusion (rate-equation) model is used to describe the processes occurring in the electrolyte and a phase-field model is used to capture microstructural evolution. This model predicts that coarsening, in which large particles grow and small ones disappear, has a substantial effect on the size distribution of the LiO₂ particles during the discharge process. The size evolution during discharge is the result of the interplay between this coarsening process and particle growth. The growth through continued deposition of LiO₂ has the effect of causing large particles to grow ever faster while delaying the dissolution of small particles. The predicted size evolution is consistent with experimental results for a previously reported cathode material based on activated carbon during discharge and when it is at rest, although kinetic factors need to be included. Finally, the approach described in this paper synergistically combines models on different length scales with experimental observations and should have applications in studying other related discharge processes, such as Li₂O₂ deposition, in Li-O₂ batteries and nucleation and growth in Li-S batteries.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1287335

Alternate ID(s):: OSTI ID: 1228788

Journal Information:: Journal of Chemical Physics, Vol. 143, Issue 22; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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