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Title: Spatial Heterogeneities and Onset of Passivation Breakdown at Lithium Anode Interfaces

Effective passivation of lithium metal surfaces, and prevention of battery-shorting lithium dendrite growth, are critical for implementing lithium metal anodes for batteries with increased power densities. Nanoscale surface heterogeneities can be “hot spots” where anode passivation breaks down. Motivated by the observation of lithium dendrites in pores and grain boundaries in all-solid batteries, we examine lithium metal surfaces covered with Li 2O and/or LiF thin films with grain boundaries in them. Electronic structure calculations show that at >0.25 V computed equilibrium overpotential Li 2O grain boundaries with sufficiently large pores can accommodate Li0 atoms which aid e– leakage and passivation breakdown. Strain often accompanies Li insertion; applying an ~1.7% strain already lowers the computed overpotential to 0.1 V. Lithium metal nanostructures as thin as 12 Å are thermodynamically favored inside cracks in Li 2O films, becoming “incipient lithium filaments”. LiF films are more resistant to lithium metal growth. Finally, the models used herein should in turn inform passivating strategies in all-solid-state batteries.
Authors:
ORCiD logo [1] ;  [2]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
Publication Date:
Report Number(s):
SAND-2017-11808J
Journal ID: ISSN 1932-7447; 658293; TRN: US1801529
Grant/Contract Number:
AC04-94AL85000; NA0003525; AC02-05CH1123; SC0001160
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 37; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE
OSTI Identifier:
1421613

Leung, Kevin, and Jungjohann, Katherine L. Spatial Heterogeneities and Onset of Passivation Breakdown at Lithium Anode Interfaces. United States: N. p., Web. doi:10.1021/acs.jpcc.7b06983.
Leung, Kevin, & Jungjohann, Katherine L. Spatial Heterogeneities and Onset of Passivation Breakdown at Lithium Anode Interfaces. United States. doi:10.1021/acs.jpcc.7b06983.
Leung, Kevin, and Jungjohann, Katherine L. 2017. "Spatial Heterogeneities and Onset of Passivation Breakdown at Lithium Anode Interfaces". United States. doi:10.1021/acs.jpcc.7b06983. https://www.osti.gov/servlets/purl/1421613.
@article{osti_1421613,
title = {Spatial Heterogeneities and Onset of Passivation Breakdown at Lithium Anode Interfaces},
author = {Leung, Kevin and Jungjohann, Katherine L.},
abstractNote = {Effective passivation of lithium metal surfaces, and prevention of battery-shorting lithium dendrite growth, are critical for implementing lithium metal anodes for batteries with increased power densities. Nanoscale surface heterogeneities can be “hot spots” where anode passivation breaks down. Motivated by the observation of lithium dendrites in pores and grain boundaries in all-solid batteries, we examine lithium metal surfaces covered with Li2O and/or LiF thin films with grain boundaries in them. Electronic structure calculations show that at >0.25 V computed equilibrium overpotential Li2O grain boundaries with sufficiently large pores can accommodate Li0 atoms which aid e– leakage and passivation breakdown. Strain often accompanies Li insertion; applying an ~1.7% strain already lowers the computed overpotential to 0.1 V. Lithium metal nanostructures as thin as 12 Å are thermodynamically favored inside cracks in Li2O films, becoming “incipient lithium filaments”. LiF films are more resistant to lithium metal growth. Finally, the models used herein should in turn inform passivating strategies in all-solid-state batteries.},
doi = {10.1021/acs.jpcc.7b06983},
journal = {Journal of Physical Chemistry. C},
number = 37,
volume = 121,
place = {United States},
year = {2017},
month = {9}
}