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Title: Lithium dendrite growth mechanisms in polymer electrolytes and prevention strategies

Abstract

Future lithium-ion batteries must use lithium metal anodes to fulfill the demands of high energy density applications with the potential to enable affordable electric cars with 350-mile range. However, dendrite growth during charging prevents the commercialization of this technology. It has been demonstrated that the presence of a compressive mechanical stress field around a dendritic protrusion prevents growth. Several techniques based on this concept, such as protective layers, externally applied pressure and solid electrolytes have been investigated by other researchers. Because of the low coulombic efficiencies associated with the stiff protective layers and high-pressure conditions, implementation of these techniques in commercial cells is complicated. Polymer-based solid electrolytes demonstrate better efficiency and capacity retention capabilities. However, dendrite growth is still possible in polymer electrolytes at higher current densities. The simulations described in this article provide guidance on the conditions under which dendrite growth is possible in polymer cells and targets for material properties needed for dendrite prevention. Increasing the elastic modulus of the electrolyte prevents the growth of dendritic protrusions in two ways: (i) higher compressive mechanical stress leads to reduced exchange current density at the protrusion peak compared to the valley, and (ii) plastic deformation of lithium metal results inmore » reduction of the height of the dendritic protrusion. A phase map is constructed, showing the range of operation (applied current) and design (electrolyte elastic modulus) parameters that corresponds to stable lithium deposition. In conclusion, it is found that increasing the yield strength of the polymer electrolyte plays a significant role in preventing dendrite growth in lithium metal anodes, providing a new avenue for further exploration.« less

Authors:
ORCiD logo [1];  [2];  [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1510742
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 19; Journal Issue: 31; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Barai, Pallab, Higa, Kenneth, and Srinivasan, Venkat. Lithium dendrite growth mechanisms in polymer electrolytes and prevention strategies. United States: N. p., 2017. Web. doi:10.1039/c7cp03304d.
Barai, Pallab, Higa, Kenneth, & Srinivasan, Venkat. Lithium dendrite growth mechanisms in polymer electrolytes and prevention strategies. United States. doi:10.1039/c7cp03304d.
Barai, Pallab, Higa, Kenneth, and Srinivasan, Venkat. Mon . "Lithium dendrite growth mechanisms in polymer electrolytes and prevention strategies". United States. doi:10.1039/c7cp03304d. https://www.osti.gov/servlets/purl/1510742.
@article{osti_1510742,
title = {Lithium dendrite growth mechanisms in polymer electrolytes and prevention strategies},
author = {Barai, Pallab and Higa, Kenneth and Srinivasan, Venkat},
abstractNote = {Future lithium-ion batteries must use lithium metal anodes to fulfill the demands of high energy density applications with the potential to enable affordable electric cars with 350-mile range. However, dendrite growth during charging prevents the commercialization of this technology. It has been demonstrated that the presence of a compressive mechanical stress field around a dendritic protrusion prevents growth. Several techniques based on this concept, such as protective layers, externally applied pressure and solid electrolytes have been investigated by other researchers. Because of the low coulombic efficiencies associated with the stiff protective layers and high-pressure conditions, implementation of these techniques in commercial cells is complicated. Polymer-based solid electrolytes demonstrate better efficiency and capacity retention capabilities. However, dendrite growth is still possible in polymer electrolytes at higher current densities. The simulations described in this article provide guidance on the conditions under which dendrite growth is possible in polymer cells and targets for material properties needed for dendrite prevention. Increasing the elastic modulus of the electrolyte prevents the growth of dendritic protrusions in two ways: (i) higher compressive mechanical stress leads to reduced exchange current density at the protrusion peak compared to the valley, and (ii) plastic deformation of lithium metal results in reduction of the height of the dendritic protrusion. A phase map is constructed, showing the range of operation (applied current) and design (electrolyte elastic modulus) parameters that corresponds to stable lithium deposition. In conclusion, it is found that increasing the yield strength of the polymer electrolyte plays a significant role in preventing dendrite growth in lithium metal anodes, providing a new avenue for further exploration.},
doi = {10.1039/c7cp03304d},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 31,
volume = 19,
place = {United States},
year = {2017},
month = {7}
}

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Works referenced in this record:

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


Nanoporous Polymer-Ceramic Composite Electrolytes for Lithium Metal Batteries
journal, September 2013

  • Tu, Zhengyuan; Kambe, Yu; Lu, Yingying
  • Advanced Energy Materials, Vol. 4, Issue 2, Article No. 1300654
  • DOI: 10.1002/aenm.201300654

Failure Analysis of Batteries Using Synchrotron-based Hard X-ray Microtomography
journal, January 2015

  • Harry, Katherine J.; Parkinson, Dilworth Y.; Balsara, Nitash P.
  • Journal of Visualized Experiments, Vol. 102, Article No. e53021
  • DOI: 10.3791/53021

Dendrite short-circuit and fuse effect on Li/polymer/Li cells
journal, July 2006