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

Horstmann, Birger and Gallant, Betar and Mitchell, Robert and Bessler, Wolfgang G. and Shao-Horn, Yang and Bazant, Martin Z. (2013) Rate-Dependent Morphology of Li2O2 Growth in Li–O2 Batteries. Journal of Physical Chemistry Letters (4), pp. 4217-4222. ACS Publications. DOI: 10.1021/jz401973c ISSN 1948-7185

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Official URL: http://pubs.acs.org/doi/abs/10.1021/jz401973c

Abstract

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 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.

Item URL in elib:https://elib.dlr.de/86095/
Document Type:Article
Title:Rate-Dependent Morphology of Li2O2 Growth in Li–O2 Batteries
Authors:
AuthorsInstitution or Email of AuthorsAuthors ORCID iD
Horstmann, Birgerbirger.horstmann (at) dlr.deUNSPECIFIED
Gallant, BetarUNSPECIFIEDUNSPECIFIED
Mitchell, RobertUNSPECIFIEDUNSPECIFIED
Bessler, Wolfgang G.wolfgang.bessler (at) hs-offenburg.deUNSPECIFIED
Shao-Horn, Yangshaohorn (at) mit.eduUNSPECIFIED
Bazant, Martin Z.bazant (at) mit.eduUNSPECIFIED
Date:14 November 2013
Journal or Publication Title:Journal of Physical Chemistry Letters
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
DOI :10.1021/jz401973c
Page Range:pp. 4217-4222
Publisher:ACS Publications
ISSN:1948-7185
Status:Published
Keywords:lithium−oxygen batteries; surface growth; electrodeposition; continuum modeling
HGF - Research field:Energy
HGF - Program:Efficient Energy Conversion and Use (old)
HGF - Program Themes:Fuel Cells (old)
DLR - Research area:Energy
DLR - Program:E EV - Energy process technology
DLR - Research theme (Project):E - Elektrochemische Prozesse (old)
Location: Stuttgart
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Deposited By: Horstmann, Birger
Deposited On:02 Dec 2013 15:14
Last Modified:10 Jan 2019 15:55

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