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Title: Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries

Abstract

We offer an explanation for how dendrite growth can be inhibited when Li metal pouch cells are subjected to external loads, even for cells using soft, thin separators. We develop a contact mechanics model for tracking Li surface and sub-surface stresses where electrodes have realistically (micron-scale) rough surfaces. Existing models examine a single, micron-scale Li metal protrusion under a fixed local current density that presses more or less conformally against a separator or stiff electrolyte. At the larger, sub-mm scales studied here, contact between the Li metal and the separator is heterogeneous and far from conformal for surfaces with realistic roughness: the load is carried at just the tallest asperities, where stresses reach tens of MPa, while most of the Li surface feels no force at all. Yet, dendrite growth is suppressed over the entire Li surface. To explain this dendrite suppression, our electrochemical/mechanics model suggests that Li avoids plating at the tips of growing Li dendrites if there is sufficient local stress; that local contact stresses there may be high enough to close separator pores so that incremental Li + ions plate elsewhere; and that creep ensures that Li protrusions are gradually flattened. These mechanisms cannot be captured bymore » single-dendrite-scale analyses.« less

Authors:
 [1];  [1];  [2];  [3];  [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6]
  1. Northwestern Univ., Evanston, IL (United States). Mechanical Engineering Dept.
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Nanoscale Sciences
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Engineering Sciences Center
  5. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1574494
Report Number(s):
SAND2019-13633J
Journal ID: ISSN 0013-4651; 681248
Grant/Contract Number:  
AC04-94AL85000; NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 166; Journal Issue: 15; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electrodeposition - modeling; batteries-lithium; electrode kinetics; electrodeposition-modeling

Citation Formats

Zhang, Xin, Wang, Q. Jane, Harrison, Katharine L., Jungjohann, Katherine, Boyce, Brad L., Roberts, Scott A., Attia, Peter M., and Harris, Stephen J. Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries. United States: N. p., 2019. Web. doi:10.1149/2.0701914jes.
Zhang, Xin, Wang, Q. Jane, Harrison, Katharine L., Jungjohann, Katherine, Boyce, Brad L., Roberts, Scott A., Attia, Peter M., & Harris, Stephen J. Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries. United States. doi:10.1149/2.0701914jes.
Zhang, Xin, Wang, Q. Jane, Harrison, Katharine L., Jungjohann, Katherine, Boyce, Brad L., Roberts, Scott A., Attia, Peter M., and Harris, Stephen J. Mon . "Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries". United States. doi:10.1149/2.0701914jes. https://www.osti.gov/servlets/purl/1574494.
@article{osti_1574494,
title = {Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries},
author = {Zhang, Xin and Wang, Q. Jane and Harrison, Katharine L. and Jungjohann, Katherine and Boyce, Brad L. and Roberts, Scott A. and Attia, Peter M. and Harris, Stephen J.},
abstractNote = {We offer an explanation for how dendrite growth can be inhibited when Li metal pouch cells are subjected to external loads, even for cells using soft, thin separators. We develop a contact mechanics model for tracking Li surface and sub-surface stresses where electrodes have realistically (micron-scale) rough surfaces. Existing models examine a single, micron-scale Li metal protrusion under a fixed local current density that presses more or less conformally against a separator or stiff electrolyte. At the larger, sub-mm scales studied here, contact between the Li metal and the separator is heterogeneous and far from conformal for surfaces with realistic roughness: the load is carried at just the tallest asperities, where stresses reach tens of MPa, while most of the Li surface feels no force at all. Yet, dendrite growth is suppressed over the entire Li surface. To explain this dendrite suppression, our electrochemical/mechanics model suggests that Li avoids plating at the tips of growing Li dendrites if there is sufficient local stress; that local contact stresses there may be high enough to close separator pores so that incremental Li+ ions plate elsewhere; and that creep ensures that Li protrusions are gradually flattened. These mechanisms cannot be captured by single-dendrite-scale analyses.},
doi = {10.1149/2.0701914jes},
journal = {Journal of the Electrochemical Society},
number = 15,
volume = 166,
place = {United States},
year = {2019},
month = {11}
}

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