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Rate-Dependent Morphology of Li2O2 Growth in Li–O2 Batteries

  • Compact solid discharge products enable energy storage devices with high gravimetric and volumetric energy densities, but solid deposits on active surfaces can disturb charge transport and induce mechanical stress. In this Letter, we develop a nanoscale continuum model for the growth of Li2O2 crystals in lithium–oxygen batteries with organic electrolytes, based on a theory of electrochemicalCompact solid discharge products enable energy storage devices with high gravimetric and volumetric energy densities, but solid deposits on active surfaces can disturb charge transport and induce mechanical stress. In this Letter, we develop a nanoscale continuum model for the growth of Li2O2 crystals in lithium–oxygen batteries with organic electrolytes, based on a theory of electrochemical nonequilibrium thermodynamics originally applied to Li-ion batteries. As in the case of lithium insertion in phase-separating LiFePO4 nanoparticles, the theory predicts a transition from complex to uniform morphologies of Li2O2 with increasing current. Discrete particle growth at low discharge rates becomes suppressed at high rates, resulting in a film of electronically insulating Li2O2 that limits cell performance. We predict that the transition between these surface growth modes occurs at current densities close to the exchange current density of the cathode reaction, consistent with experimental observations.show moreshow less

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Metadaten
Author:Birger Horstmann, Betar Gallant, Robert Mitchell, Wolfgang G. BesslerORCiDGND, Yang Shao-Horn, Martin Z. Bazant
Creating Corporation:American Chemical Society
Year of Publication:2013
Language:English
GND Keyword:Lithium; Lithiumbatterie; Morphologie
Parent Title (English):The Journal of Physical Chemistry Letters
Volume:4
Issue:24
ISSN:1948-7185
First Page:4217
Last Page:4222
Document Type:Article (reviewed)
Institutes:Hochschule Offenburg / Bibliografie
Acces Right:Frei zugänglich
Release Date:2018/03/06
Licence (German):License LogoEs gilt das UrhG
DOI:https://doi.org/10.1021/jz401973c
ArXiv Id:http://arxiv.org/abs/1307.6621
Pubmed Id:http://www.ncbi.nlm.nih.gov/pubmed?term=26296168