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:
-
- Univ. of Notre Dame, IN (United States). Dept. of Chemical and Biomolecular Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Div.
- Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education
- Worcester Polytechnic Institute, MA (United States). Dept. of Mechanical Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- 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}
}
Works referenced in this record:
Dual‐Phase Single‐Ion Pathway Interfaces for Robust Lithium Metal in Working Batteries
journal, March 2019
- Xu, Rui; Xiao, Ye; Zhang, Rui
- Advanced Materials, Vol. 31, Issue 19
Determining and Minimizing Resistance for Ion Transport at the Polymer/Ceramic Electrolyte Interface
journal, April 2019
- Chen, X. Chelsea; Liu, Xiaoming; Samuthira Pandian, Amaresh
- ACS Energy Letters, Vol. 4, Issue 5
Relationship between Ion Dissociation, Melt Morphology, and Electrochemical Performance of Lithium and Magnesium Single-Ion Conducting Block Copolymers
journal, November 2016
- Thelen, Jacob L.; Inceoglu, Sebnem; Venkatesan, Naveen R.
- Macromolecules, Vol. 49, Issue 23
Promising Routes to a High Li + Transference Number Electrolyte for Lithium Ion Batteries
journal, October 2017
- Diederichsen, Kyle M.; McShane, Eric J.; McCloskey, Bryan D.
- ACS Energy Letters, Vol. 2, Issue 11
Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material
journal, January 2019
- Zhang, Yubin; Zheng, Zhangfeng; Liu, Xiaoming
- Journal of The Electrochemical Society, Vol. 166, Issue 4
The pursuit of solid-state electrolytes for lithium batteries: from comprehensive insight to emerging horizons
journal, January 2016
- Chen, Renjie; Qu, Wenjie; Guo, Xing
- Materials Horizons, Vol. 3, Issue 6
Single Lithium-Ion Conducting Polymer Electrolytes Based on a Super-Delocalized Polyanion
journal, January 2016
- Ma, Qiang; Zhang, Heng; Zhou, Chongwang
- Angewandte Chemie International Edition, Vol. 55, Issue 7
A Nuclear Magnetic Resonance Study of Cation and Anion Dynamics in Polymer–Ceramic Composite Solid Electrolytes
journal, March 2020
- Peng, Jing; Xiao, Ye; Clarkson, David A.
- ACS Applied Polymer Materials, Vol. 2, Issue 3
Toward Critical Electrode/Electrolyte Interfaces in Rechargeable Batteries
journal, April 2020
- Yan, Chong; Xu, Rui; Xiao, Ye
- Advanced Functional Materials, Vol. 30, Issue 23
Ionic Conduction in Composite Polymer Electrolytes: Case of PEO:Ga-LLZO Composites
journal, December 2018
- Li, Zhuo; Huang, He-Ming; Zhu, Jia-Kun
- ACS Applied Materials & Interfaces, Vol. 11, Issue 1
Role of the ceramic fillers in enhancing the transport properties of composite polymer electrolytes
journal, May 2001
- Croce, F.; Persi, L.; Scrosati, B.
- Electrochimica Acta, Vol. 46, Issue 16
Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering
journal, January 2019
- Chen, X. Chelsea; Sacci, Robert L.; Osti, Naresh C.
- Molecular Systems Design & Engineering, Vol. 4, Issue 2
Application of Single-Ion Conducting Gel Polymer Electrolytes in Magnesium Batteries
journal, August 2019
- Merrill, Laura C.; Ford, Hunter O.; Schaefer, Jennifer L.
- ACS Applied Energy Materials, Vol. 2, Issue 9
Amorphous LiLaTiO 3 as Solid Electrolyte Material
journal, January 2014
- Zheng, Zhangfeng; Fang, Huazhi; Yang, Fan
- Journal of The Electrochemical Society, Vol. 161, Issue 4
UV-Cross-Linked Composite Polymer Electrolyte for High-Rate, Ambient Temperature Lithium Batteries
journal, February 2019
- Falco, Marisa; Castro, Laurent; Nair, Jijeesh Ravi
- ACS Applied Energy Materials, Vol. 2, Issue 3
Lithiated Nafion-garnet ceramic composite electrolyte membrane for solid-state lithium metal battery
journal, July 2020
- Gao, Jing; Shao, Qinjun; Chen, Jian
- Journal of Energy Chemistry, Vol. 46
Single-ion polymer electrolytes based on a delocalized polyanion for lithium batteries
journal, December 2011
- Meziane, Rachid; Bonnet, Jean-Pierre; Courty, Matthieu
- Electrochimica Acta, Vol. 57
Spectroscopic characterization of the conformational states of the bis(trifluoromethanesulfonyl)imide anion (TFSI−)
journal, January 2005
- Herstedt, M.; Smirnov, M.; Johansson, P.
- Journal of Raman Spectroscopy, Vol. 36, Issue 8
Ion Transport in Solvent-Free, Crosslinked, Single-Ion Conducting Polymer Electrolytes for Post-Lithium Ion Batteries
journal, June 2018
- Elmore, Clay; Seidler, Morgan; Ford, Hunter
- Batteries, Vol. 4, Issue 2
Synergistic Coupling between Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 and Poly(vinylidene fluoride) Induces High Ionic Conductivity, Mechanical Strength, and Thermal Stability of Solid Composite Electrolytes
journal, September 2017
- Zhang, Xue; Liu, Ting; Zhang, Shuofeng
- Journal of the American Chemical Society, Vol. 139, Issue 39
Sol–gel-processed amorphous inorganic lithium ion electrolyte thin films: sol chemistry
journal, January 2017
- Zheng, Zhangfeng; Zhang, Yubin; Song, Shidong
- RSC Advances, Vol. 7, Issue 48
Review on composite polymer electrolytes for lithium batteries
journal, July 2006
- Manuel Stephan, A.; Nahm, K. S.
- Polymer, Vol. 47, Issue 16
A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte
journal, April 2020
- Palmer, Max J.; Kalnaus, Sergiy; Dixit, Marm B.
- Energy Storage Materials, Vol. 26
Simultaneously Enhancing the Thermal Stability, Mechanical Modulus, and Electrochemical Performance of Solid Polymer Electrolytes by Incorporating 2D Sheets
journal, June 2018
- Tang, Wenjing; Tang, Shan; Zhang, Cuijuan
- Advanced Energy Materials, Vol. 8, Issue 24
Charging toward improved lithium-ion polymer electrolytes: exploiting synergistic experimental and computational approaches to facilitate materials design
journal, January 2019
- Ketkar, Priyanka M.; Shen, Kuan-Hsuan; Hall, Lisa M.
- Molecular Systems Design & Engineering, Vol. 4, Issue 2
Ion Association and Ion Solvation Effects at the Crystalline−Amorphous Phase Transition in PEO−LiTFSI
journal, August 2000
- Edman, Ludvig
- The Journal of Physical Chemistry B, Vol. 104, Issue 31
Review—On Order and Disorder in Polymer Electrolytes
journal, January 2015
- Golodnitsky, D.; Strauss, E.; Peled, E.
- Journal of The Electrochemical Society, Vol. 162, Issue 14
Single-ion Polyelectrolyte/ Mesoporous Hollow-Silica Spheres, Composite Electrolyte Membranes for Lithium-ion Batteries
journal, November 2015
- Yu, Qingchun; Nie, Yu; Cui, Yao
- Electrochimica Acta, Vol. 182
A Fundamental Stability Study for Amorphous LiLaTiO 3 Solid Electrolyte
journal, November 2014
- Zheng, Zhangfeng; Fang, Hua-zhi; Liu, Zi-kui
- Journal of The Electrochemical Society, Vol. 162, Issue 1
High‐Performance Solid Polymer Electrolytes Filled with Vertically Aligned 2D Materials
journal, February 2019
- Tang, Wenjing; Tang, Shan; Guan, Xuze
- Advanced Functional Materials, Vol. 29, Issue 16
Beyond Intercalation-Based Li-Ion Batteries: The State of the Art and Challenges of Electrode Materials Reacting Through Conversion Reactions
journal, August 2010
- Cabana, Jordi; Monconduit, Laure; Larcher, Dominique
- Advanced Materials, Vol. 22, Issue 35
Enhanced Li + Conduction within Single-Ion Conducting Polymer Gel Electrolytes via Reduced Cation–Polymer Interaction
journal, February 2020
- Ford, Hunter O.; Park, Bumjun; Jiang, Jizhou
- ACS Materials Letters, Vol. 2, Issue 3
UV-cured methacrylate based polymer composite electrolyte for metallic lithium batteries
journal, March 2019
- Amici, J.; Romanin, S.; Alidoost, M.
- Journal of Electroanalytical Chemistry, Vol. 837
Nanoporous Polymer Films with a High Cation Transference Number Stabilize Lithium Metal Anodes in Light-Weight Batteries for Electrified Transportation
journal, January 2019
- Ma, Lin; Fu, Chengyin; Li, Longjun
- Nano Letters, Vol. 19, Issue 2
Highly Conductive, Sulfonated, UV-Cross-Linked Separators for Li–S Batteries
journal, July 2016
- Ma, Lin; Nath, Pooja; Tu, Zhengyuan
- Chemistry of Materials, Vol. 28, Issue 14
Increased ion conduction in dual cation [sodium][tetraalkylammonium] poly[4-styrenesulfonyl(trifluoromethylsulfonyl)imide-co-ethylacrylate] ionomers
journal, January 2015
- Li, Jiaye; Zhu, Haijin; Wang, Xiaoen
- Journal of Materials Chemistry A, Vol. 3, Issue 39
The energy-storage frontier: Lithium-ion batteries and beyond
journal, November 2015
- Crabtree, George; Kócs, Elizabeth; Trahey, Lynn
- MRS Bulletin, Vol. 40, Issue 12
Sol-gel-processed amorphous lithium ion electrolyte thin films: Structural evolution, theoretical considerations, and ion transport processes
journal, April 2016
- Zheng, Zhangfeng; Song, Shidong; Wang, Yan
- Solid State Ionics, Vol. 287
Electrochemical measurement of transference numbers in polymer electrolytes
journal, December 1987
- Evans, James; Vincent, Colin A.; Bruce, Peter G.
- Polymer, Vol. 28, Issue 13
Stable Conversion Chemistry-Based Lithium Metal Batteries Enabled by Hierarchical Multifunctional Polymer Electrolytes with Near-Single Ion Conduction
journal, March 2019
- Zhou, Dong; Tkacheva, Anastasia; Tang, Xiao
- Angewandte Chemie International Edition, Vol. 58, Issue 18
Design of composite polymer electrolytes for Li ion batteries based on mechanical stability criteria
journal, March 2012
- Kalnaus, Sergiy; Sabau, Adrian S.; Tenhaeff, Wyatt E.
- Journal of Power Sources, Vol. 201
Hybrid electrolytes for lithium metal batteries
journal, July 2018
- Keller, Marlou; Varzi, Alberto; Passerini, Stefano
- Journal of Power Sources, Vol. 392
A Single‐Ion Conducting Borate Network Polymer as a Viable Quasi‐Solid Electrolyte for Lithium Metal Batteries
journal, January 2020
- Shin, Dong‐Myeong; Bachman, Jonathan E.; Taylor, Mercedes K.
- Advanced Materials, Vol. 32, Issue 10
Enhancing the ionic conductivity in a composite polymer electrolyte with ceramic nanoparticles anchored to charged polymer brushes
journal, March 2020
- Zhao, Bintao; Lu, Xi; Wang, Qian
- Chinese Chemical Letters, Vol. 31, Issue 3
Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings
journal, June 2018
- Pandian, Amaresh Samuthira; Chen, X. Chelsea; Chen, Jihua
- Journal of Power Sources, Vol. 390
Nanocomposite polymer electrolyte for rechargeable magnesium batteries
journal, March 2015
- Shao, Yuyan; Rajput, Nav Nidhi; Hu, Jianzhi
- Nano Energy, Vol. 12