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This content will become publicly available on September 8, 2018

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.
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):
Journal ID: ISSN 1932-7447; 658293
Grant/Contract Number:
AC04-94AL85000; NA0003525; AC02-05CH1123; SC0001160
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 37; Journal ID: ISSN 1932-7447
American Chemical Society
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
OSTI Identifier: