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

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/c7cp03304d· OSTI ID:1510742
ORCiD logo [1];  [2];  [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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. 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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE) - Office of Vehicle Technologies (VTO) - Battery Materials Research (BMR) Program
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357
OSTI ID:
1510742
Alternate ID(s):
OSTI ID: 1671339
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 19, Issue 31; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 209 works
Citation information provided by
Web of Science

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Electrode Edge Effects and the Failure Mechanism of Lithium-Metal Batteries journal October 2018
An Aggregate Cluster-Dispersed Electrolyte Guides the Uniform Nucleation and Growth of Lithium at Lithium Metal Anodes journal November 2018
Cationic shield mediated electrodeposition stability in metal electrodes journal January 2019
Lithium Mechanics: Roles of Strain Rate and Temperature and Implications for Lithium Metal Batteries journal January 2019
Metal Electrode Surfaces Can Roughen Despite the Constraint of a Stiff Electrolyte journal January 2019
Impact of External Pressure and Electrolyte Transport Properties on Lithium Dendrite Growth journal January 2018
On our Limited Understanding of Electrodeposition journal January 2019
The influence of stress field on Li electrodeposition in Li-metal battery journal July 2018
Solvent-Free and Scalable Procedure to Prepare PYR13TFSI/LiTFSI/PVDF–HFP Thermoplastic Electrolytes with Controlled Phase Separation and Enhanced Li Ion Diffusion journal April 2019