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Title: Polymer–Ceramic Composite Electrolytes for Lithium Batteries: A Comparison between the Single-Ion-Conducting Polymer Matrix and Its Counterpart

Abstract

Single-ion-conducting polymer electrolytes are attractive to use in lithium batteries as the transference number of the lithium cation approaches unity. This helps prevent concentration gradients across the electrolyte, which can result in dendrite formation. The addition of ceramic particles to polymer electrolytes at high loadings can increase the mechanical strength of the polymer, which can also help suppress dendrite formation. Here, a single-ion-conducting polymer electrolyte is blended with lithium-conducting oxide ceramic particles to make a composite electrolyte. This electrolyte is studied in comparison to a composite electrolyte containing freely dissolved lithium salt. It is found that the addition of ceramic particles to the single-ion-conducting polymer can result in increased cation dissociation and consequent increased ionic conductivity. The electrolytes are cycled in lithium symmetrical cells, and it is found that the ceramic-containing electrolytes show increased interfacial stability with the lithium metal compared to the pristine polymer electrolytes. Our findings shed light on how to optimize the polymer host chemistry to form composite electrolytes that can meet the challenging requirements to stabilize the lithium metal anode.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [1];  [6]
  1. Univ. of Notre Dame, IN (United States). Dept. of Chemical and Biomolecular Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Div.
  3. Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education
  4. Worcester Polytechnic Institute, MA (United States). Dept. of Mechanical Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
  6. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1783052
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Energy Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2574-0962
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; composite; polymer, ceramic; lithium; battery; single-ion conducting; electrolyte

Citation Formats

Merrill, Laura C., Chen, Xi Chelsea, Zhang, Yiman, Ford, Hunter O., Lou, Kun, Zhang, Yubin, Yang, Guang, Wang, Yangyang, Wang, Yan, Schaefer, Jennifer L., and Dudney, Nancy J. Polymer–Ceramic Composite Electrolytes for Lithium Batteries: A Comparison between the Single-Ion-Conducting Polymer Matrix and Its Counterpart. United States: N. p., 2020. Web. doi:10.1021/acsaem.0c01358.
Merrill, Laura C., Chen, Xi Chelsea, Zhang, Yiman, Ford, Hunter O., Lou, Kun, Zhang, Yubin, Yang, Guang, Wang, Yangyang, Wang, Yan, Schaefer, Jennifer L., & Dudney, Nancy J. Polymer–Ceramic Composite Electrolytes for Lithium Batteries: A Comparison between the Single-Ion-Conducting Polymer Matrix and Its Counterpart. United States. https://doi.org/10.1021/acsaem.0c01358
Merrill, Laura C., Chen, Xi Chelsea, Zhang, Yiman, Ford, Hunter O., Lou, Kun, Zhang, Yubin, Yang, Guang, Wang, Yangyang, Wang, Yan, Schaefer, Jennifer L., and Dudney, Nancy J. Wed . "Polymer–Ceramic Composite Electrolytes for Lithium Batteries: A Comparison between the Single-Ion-Conducting Polymer Matrix and Its Counterpart". United States. https://doi.org/10.1021/acsaem.0c01358. https://www.osti.gov/servlets/purl/1783052.
@article{osti_1783052,
title = {Polymer–Ceramic Composite Electrolytes for Lithium Batteries: A Comparison between the Single-Ion-Conducting Polymer Matrix and Its Counterpart},
author = {Merrill, Laura C. and Chen, Xi Chelsea and Zhang, Yiman and Ford, Hunter O. and Lou, Kun and Zhang, Yubin and Yang, Guang and Wang, Yangyang and Wang, Yan and Schaefer, Jennifer L. and Dudney, Nancy J.},
abstractNote = {Single-ion-conducting polymer electrolytes are attractive to use in lithium batteries as the transference number of the lithium cation approaches unity. This helps prevent concentration gradients across the electrolyte, which can result in dendrite formation. The addition of ceramic particles to polymer electrolytes at high loadings can increase the mechanical strength of the polymer, which can also help suppress dendrite formation. Here, a single-ion-conducting polymer electrolyte is blended with lithium-conducting oxide ceramic particles to make a composite electrolyte. This electrolyte is studied in comparison to a composite electrolyte containing freely dissolved lithium salt. It is found that the addition of ceramic particles to the single-ion-conducting polymer can result in increased cation dissociation and consequent increased ionic conductivity. The electrolytes are cycled in lithium symmetrical cells, and it is found that the ceramic-containing electrolytes show increased interfacial stability with the lithium metal compared to the pristine polymer electrolytes. Our findings shed light on how to optimize the polymer host chemistry to form composite electrolytes that can meet the challenging requirements to stabilize the lithium metal anode.},
doi = {10.1021/acsaem.0c01358},
journal = {ACS Applied Energy Materials},
number = 9,
volume = 3,
place = {United States},
year = {Wed Sep 16 00:00:00 EDT 2020},
month = {Wed Sep 16 00:00:00 EDT 2020}
}

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