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Title: Effect of Initial State of Lithium on the Propensity for Dendrite Formation: A Theoretical Study

Mechanical constraints have been widely used experimentally to prevent the growth of dendrites within lithium metal. The only article known to the authors that tries to theoretically understand how mechanical forces prevent dendrite growth was published by Monroe and Newman [J. Electrochem. Soc., 150 (10) A1377 (2005)]. Based on the assumption that surface tension prevents the growth of interfacial roughness, Monroe and Newman considered pre-stressed conditions of the lithium electrodes. This scenario indicates that prevention of dendrite growth by mechanical means is only possible by using electrolytes with shear modulus at least two times larger than that of lithium metal. Here, a different scenario of relaxed lithium metal (without any pre-existing surface stresses) has been considered in the present analysis. Deposition of lithium due to electrochemical reaction at the lithium/electrolyte interface induces compressive stress at the electrode, the electrolyte, and the newly deposited lithium metal. Present simulations indicate that during operation at low current densities, the scenario of relaxed lithium leads to no dendrites. Rather, the present study points to the importance of including the effect of current distribution to accurately capture the mechanical forces needed to prevent dendrite growth.
Authors:
 [1] ;  [1] ;  [1]
  1. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 2; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; dendrite growth; effective exchange current density; lithium metal anode; mechanical stress
OSTI Identifier:
1436144

Barai, Pallab, Higa, Kenneth, and Srinivasan, Venkat. Effect of Initial State of Lithium on the Propensity for Dendrite Formation: A Theoretical Study. United States: N. p., Web. doi:10.1149/2.0661702jes.
Barai, Pallab, Higa, Kenneth, & Srinivasan, Venkat. Effect of Initial State of Lithium on the Propensity for Dendrite Formation: A Theoretical Study. United States. doi:10.1149/2.0661702jes.
Barai, Pallab, Higa, Kenneth, and Srinivasan, Venkat. 2016. "Effect of Initial State of Lithium on the Propensity for Dendrite Formation: A Theoretical Study". United States. doi:10.1149/2.0661702jes. https://www.osti.gov/servlets/purl/1436144.
@article{osti_1436144,
title = {Effect of Initial State of Lithium on the Propensity for Dendrite Formation: A Theoretical Study},
author = {Barai, Pallab and Higa, Kenneth and Srinivasan, Venkat},
abstractNote = {Mechanical constraints have been widely used experimentally to prevent the growth of dendrites within lithium metal. The only article known to the authors that tries to theoretically understand how mechanical forces prevent dendrite growth was published by Monroe and Newman [J. Electrochem. Soc., 150 (10) A1377 (2005)]. Based on the assumption that surface tension prevents the growth of interfacial roughness, Monroe and Newman considered pre-stressed conditions of the lithium electrodes. This scenario indicates that prevention of dendrite growth by mechanical means is only possible by using electrolytes with shear modulus at least two times larger than that of lithium metal. Here, a different scenario of relaxed lithium metal (without any pre-existing surface stresses) has been considered in the present analysis. Deposition of lithium due to electrochemical reaction at the lithium/electrolyte interface induces compressive stress at the electrode, the electrolyte, and the newly deposited lithium metal. Present simulations indicate that during operation at low current densities, the scenario of relaxed lithium leads to no dendrites. Rather, the present study points to the importance of including the effect of current distribution to accurately capture the mechanical forces needed to prevent dendrite growth.},
doi = {10.1149/2.0661702jes},
journal = {Journal of the Electrochemical Society},
number = 2,
volume = 164,
place = {United States},
year = {2016},
month = {12}
}

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Lithium metal stripping/plating mechanisms studies: A metallurgical approach
journal, October 2006

Failure Analysis of Batteries Using Synchrotron-based Hard X-ray Microtomography
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