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

An atomistically informed mesoscale model is developed for the deposition of a discharge product in a Li-O{sub 2} battery. This mescocale model includes particle growth and coarsening as well as a simplified nucleation model. The model involves LiO{sub 2} formation through reaction of O{sub 2}{sup −} and Li{sup +} in the electrolyte, which deposits on the cathode surface when the LiO{sub 2} 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 LiO{sub 2} 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 LiO{sub 2} 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 bemore » included. 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 Li{sub 2}O{sub 2} deposition, in Li-O{sub 2} batteries and nucleation and growth in Li-S batteries.« less
Authors:
; ; ; ;  [1] ;  [2] ;  [3]
  1. Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439 (United States)
  2. Mathematics and Computer Science, Argonne National Laboratory, Argonne, Illinois 60439 (United States)
  3. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439 (United States)
Publication Date:
OSTI Identifier:
22493306
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 22; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ACTIVATED CARBON; CATHODES; CONCENTRATION RATIO; DEPOSITION; DIFFUSION; DISSOLUTION; ELECTROLYTES; EV RANGE; EVOLUTION; LITHIUM; LITHIUM IONS; LITHIUM OXIDES; MICROSTRUCTURE; NUCLEATION; OXYGEN; PARTICLES; REACTION KINETICS; SUPERSATURATION