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Gel composite electrolyte – an effective way to utilize ceramic fillers in lithium batteries

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/d1ta00180a· OSTI ID:1783046
 [1];  [1];  [2];  [1];  [3];  [2];  [4];  [5];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Div.
  2. Univ. of Notre Dame, IN (United States). Dept. of Chemical and Biomolecular Engineering
  3. Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Div.
  5. 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

Achieving synergy between ion-conducting polymers and ceramics in a composite electrolyte has been proven to be difficult as the complicated ceramic/polymer interface presents challenges to understand and control. In this work, we report a strategy to utilize discrete ceramic fillers to form a gel composite electrolyte with enhanced transport properties for lithium metal batteries. The matrix of the composite membrane is crosslinked poly(ethylene oxide) with bis(trifluoromethane)sulfonimide lithium salt (LiTFSI). The membrane is plasticized with tetraethylene glycol dimethyl ether (TEGDME). The incorporation of doped-lithium aluminum titanium phosphate particles (LICGC™) into the membrane greatly improves the membrane's cycling characteristics against the lithium electrode, exhibiting lower interfacial impedance, lower overpotential and higher rate capability. The underpinnings of the superior performance of the gel composite electrolyte are discussed in depth. LICGC™ can immobilize the TFSI- anions in the polymer matrix and simultaneously promote Li+ transport by increasing the plasticizer to Li+ ratio. Further, the transport enhancement is achieved without sacrificing mechanical properties. The composite membrane shows significantly improved handleability and processability. This work sheds light on the design strategy for a safe electrolyte towards stable Li metal batteries.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office. Batteries for Advanced Transportation Technologies (BATT) Program
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1783046
Alternate ID(s):
OSTI ID: 1766114
Journal Information:
Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 10 Vol. 9; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (48)

Flexible, Scalable, and Highly Conductive Garnet-Polymer Solid Electrolyte Templated by Bacterial Cellulose journal March 2018
Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries journal December 2016
Complexes of alkali metal ions with poly(ethylene oxide) journal November 1973
Electrochemical measurement of transference numbers in polymer electrolytes journal December 1987
A new Na+ ion conducting polymer electrolyte based on (PEO+NaYF4) and its use as an electrochemical cell journal December 1994
Experimental investigations on a sodium-ion-conducting polymer electrolyte based on poly(ethylene oxide) complexed with NaPF6 journal October 1995
Characteristics of lithium-ion-conducting composite polymer-glass secondary cell electrolytes journal October 2002
Tailored crosslinking of Poly(ethylene oxide) enables mechanical robustness and improved sodium-ion conductivity journal September 2019
A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte journal April 2020
Lithiated Nafion-garnet ceramic composite electrolyte membrane for solid-state lithium metal battery journal July 2020
The effect of type of the inorganic filler and dopant salt concentration on the PEO–LiClO4 based composite electrolyte–lithium electrode interfacial resistivity journal September 2006
Advanced, high-performance composite polymer electrolytes for lithium batteries journal October 2006
Composite PEOn:NaTFSI polymer electrolyte: Preparation, thermal and electrochemical characterization journal February 2014
Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings journal June 2018
Hybrid electrolytes for lithium metal batteries journal July 2018
PEO/garnet composite electrolytes for solid-state lithium batteries: From “ceramic-in-polymer” to “polymer-in-ceramic” journal April 2018
Beyond PEO—Alternative host materials for Li + -conducting solid polymer electrolytes journal June 2018
Microstructure and temperature dependent lithium ion transport of ceramic–polymer composite electrolyte for solid-state lithium ion batteries based on garnet-type Li7La3Zr2O12 journal August 2016
Gel polymer electrolytes for lithium ion batteries: Fabrication, characterization and performance journal May 2018
Effect of Plasticization on Ionic Conductivity Enhancement in Relation to Glass Transition Temperature of Crosslinked Polymer Electrolyte Membranes journal July 2016
Ionic Conductivity Enhancement of Polymer Electrolytes with Ceramic Nanowire Fillers journal March 2015
Polymer–Ceramic Composite Electrolytes for Lithium Batteries: A Comparison between the Single-Ion-Conducting Polymer Matrix and Its Counterpart journal September 2020
Composite Polymer Electrolytes with Li 7 La 3 Zr 2 O 12 Garnet-Type Nanowires as Ceramic Fillers: Mechanism of Conductivity Enhancement and Role of Doping and Morphology journal June 2017
Scalable Freeze-Tape-Casting Fabrication and Pore Structure Analysis of 3D LLZO Solid-State Electrolytes journal December 2019
A Nuclear Magnetic Resonance Study of Cation and Anion Dynamics in Polymer–Ceramic Composite Solid Electrolytes journal March 2020
Single-Ion Conducting Polymer Electrolytes for Lithium Metal Polymer Batteries that Operate at Ambient Temperature journal September 2016
Determining and Minimizing Resistance for Ion Transport at the Polymer/Ceramic Electrolyte Interface journal April 2019
Suppression of Lithium Dendrite Growth Using Cross-Linked Polyethylene/Poly(ethylene oxide) Electrolytes: A New Approach for Practical Lithium-Metal Polymer Batteries journal May 2014
Ion Association and Ion Solvation Effects at the Crystalline−Amorphous Phase Transition in PEO−LiTFSI journal August 2000
Glass Transition of Polymer−Nanocrystal Thin Film Mixtures: Role of Entropically Directed Forces on Nanocrystal Distribution journal August 2008
Enhancing ionic conductivity in composite polymer electrolytes with well-aligned ceramic nanowires journal April 2017
Poly(Ethylene Oxide)-based Electrolyte for Solid-State-Lithium-Batteries with High Voltage Positive Electrodes: Evaluating the Role of Electrolyte Oxidation in Rapid Cell Failure journal March 2020
Lithium metal anodes for rechargeable batteries journal January 2014
Li 0.33 La 0.557 TiO 3 ceramic nanofiber-enhanced polyethylene oxide-based composite polymer electrolytes for all-solid-state lithium batteries journal January 2018
Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering journal January 2019
A dopamine modified Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 /PEO solid-state electrolyte: enhanced thermal and electrochemical properties journal January 2019
Flexible, solid-state, ion-conducting membrane with 3D garnet nanofiber networks for lithium batteries journal June 2016
Fast Ionic Transport in Solids journal June 1979
Handbook of Solid State Batteries book January 2015
Polymer Electrolytes journal July 2013
Polymer Electrolytes journal August 1986
Investigation on the Stability of the Lithium-Polymer Electrolyte Interface journal January 2000
Well-designed Crosslinked Polymer Electrolyte Enables High Ionic Conductivity and Enhanced Salt Solvation journal January 2020
Impedance Spectroscopy Analysis of the Lithium Ion Transport through the Li 7 La 3 Zr 2 O 12 /P(EO) 20 Li Interface journal January 2017
Comparing Cycling Characteristics of Symmetric Lithium-Polymer-Lithium Cells with Theoretical Predictions journal January 2018
Controlling Ionic Transport through the PEO-LiTFSI/LLZTO Interface journal January 2019
Study of the Segmental Dynamics and Ion Transport of Solid Polymer Electrolytes in the Semi-crystalline State journal January 2021
Recent Developments and Challenges in Hybrid Solid Electrolytes for Lithium-Ion Batteries journal September 2020

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