DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Designing solvate ionogel electrolytes with very high room-temperature conductivity and lithium transference number

Journal Article · · Journal of Materials Chemistry. A
DOI: https://doi.org/10.1039/c8ta08808j · OSTI ID:1491354

Here, free-standing electrolytes based on Li(G4)TFSI and chemically-crosslinked poly(ethylene glycol), as well as functional co-monomers and/or small amounts of volatile diluent, are demonstrated to reach very high room-temperature ionic conductivities (>2 × 10–3 S cm–1) and electrochemically-measured lithium transference numbers (>0.5). An unexpected dependence of properties on polymer length/crosslinking is observed and explained in terms of competing Li+ transport processes. These electrolytes enable lithium symmetric cells to cycle >600 h at low overpotential and without dendrite growth. Future optimization routes are also discussed.

Research Organization:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
EE0007791
OSTI ID:
1491354
Journal Information:
Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 47 Vol. 6; ISSN JMCAET; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (67)

Ionic Liquid-Nanoparticle Hybrid Electrolytes and their Application in Secondary Lithium-Metal Batteries journal July 2012
Preparation of High-Performance Ionogels with Excellent Transparency, Good Mechanical Strength, and High Conductivity journal October 2017
High Energy Density Lithium-Sulfur Batteries: Challenges of Thick Sulfur Cathodes journal March 2015
Ionic-Liquid-Nanoparticle Hybrid Electrolytes: Applications in Lithium Metal Batteries journal November 2013
On the elastic modulus of swollen gels journal June 1987
Electrochemical measurement of transference numbers in polymer electrolytes journal December 1987
Polymer gels journal October 1981
On the origin and application of the Bruggeman correlation for analysing transport phenomena in electrochemical systems journal May 2016
Vinylene carbonate–LiNO3: A hybrid additive in carbonic ester electrolytes for SEI modification on Li metal anode journal February 2015
Li+ Ion Transport in Polymer Electrolytes Based on a Glyme-Li Salt Solvate Ionic Liquid journal September 2015
Highly efficient gel polymer electrolytes for all solid-state electrochemical charge storage devices journal July 2018
Ternary polymer electrolytes containing pyrrolidinium-based polymeric ionic liquids for lithium batteries journal June 2010
Novel dual-salts electrolyte solution for dendrite-free lithium-metal based rechargeable batteries with high cycle reversibility journal December 2014
Review on solid electrolytes for all-solid-state lithium-ion batteries journal June 2018
Truly solid state electrochromic devices constructed from polymeric ionic liquids as solid electrolytes and electrodes formulated by vapor phase polymerization of 3,4-ethylenedioxythiophene journal August 2014
Effect of molecular weight on conductivity of polymer electrolytes journal November 2011
Polymer Electrolytes Containing Solvate Ionic Liquids: A New Approach To Achieve High Ionic Conductivity, Thermal Stability, and a Wide Potential Window journal December 2017
Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review journal July 2017
Enhanced Lithium Ion Transport in Poly(ethylene glycol) Diacrylate-Supported Solvate Ionogel Electrolytes via Chemically Cross-linked Ethylene Oxide Pathways journal January 2017
Li + Solvation and Ionic Transport in Lithium Solvate Ionic Liquids Diluted by Molecular Solvents journal December 2015
Interfacial Challenges in Solid-State Li Ion Batteries journal October 2015
Relationship between Conductivity, Ion Diffusion, and Transference Number in Perfluoropolyether Electrolytes journal April 2016
Effect of Plasticization on Ionic Conductivity Enhancement in Relation to Glass Transition Temperature of Crosslinked Polymer Electrolyte Membranes journal July 2016
Homogeneous Lithium Electrodeposition with Pyrrolidinium-Based Ionic Liquid Electrolytes journal March 2015
Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy journal October 2016
Promising Routes to a High Li + Transference Number Electrolyte for Lithium Ion Batteries journal October 2017
Controversial Topics on Lithium Superoxide in Li–O 2 Batteries journal November 2017
Highly Conductive PEO-like Polymer Electrolytes journal September 1997
Electrolytes and Interphases in Li-Ion Batteries and Beyond journal October 2014
Chelate ring size and metal ion selection. The basis of selectivity for metal ions in open-chain ligands and macrocycles journal August 1992
Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism journal March 2013
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
Effect of Water and Organic Solvents on the Ionic Dissociation of Ionic Liquids journal June 2007
Change from Glyme Solutions to Quasi-ionic Liquids for Binary Mixtures Consisting of Lithium Bis(trifluoromethanesulfonyl)amide and Glymes journal August 2011
Glyme–Lithium Salt Equimolar Molten Mixtures: Concentrated Solutions or Solvate Ionic Liquids? journal August 2012
Chelate Effects in Glyme/Lithium Bis(trifluoromethanesulfonyl)amide Solvate Ionic Liquids. I. Stability of Solvate Cations and Correlation with Electrolyte Properties journal May 2014
Enhanced Lithium Transference Numbers in Ionic Liquid Electrolytes journal October 2008
A Molecular Theory of Polymer Gels journal February 2002
Microscopic Definition of Polymer Entanglements journal February 2014
Gelation of Solvate Ionic Liquid by Self-Assembly of Block Copolymer and Characterization as Polymer Electrolyte journal August 2014
Elastic Modulus and Equilibrium Swelling of Polyelectrolyte Gels journal January 1996
A highly reversible room-temperature lithium metal battery based on crosslinked hairy nanoparticles journal December 2015
A reversible dendrite-free high-areal-capacity lithium metal electrode journal April 2017
A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries journal February 2013
Design principles for electrolytes and interfaces for stable lithium-metal batteries journal September 2016
Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes journal September 2016
Stable lithium electrodeposition in liquid and nanoporous solid electrolytes journal August 2014
Reviving the lithium metal anode for high-energy batteries journal March 2017
Ionic semi-interpenetrating networks as a new approach for highly conductive and stretchable polymer materials journal January 2015
Conformation of poly(ethylene oxide) dissolved in the solvate ionic liquid [Li(G4)]TFSI journal January 2015
On the concept of ionicity in ionic liquids journal January 2009
Transport properties of ionic liquid electrolytes with organic diluents journal January 2009
Ionic conductivity, glass transition, and local free volume in poly(ethylene oxide) electrolytes: Single and mixed ion conductors journal May 2003
Molecular dynamics study of thermodynamic stability and dynamics of [Li(glyme)]+ complex in lithium-glyme solvate ionic liquids journal January 2018
Composite lithium metal anode by melt infusion of lithium into a 3D conducting scaffold with lithiophilic coating journal February 2016
Three-dimensional stable lithium metal anode with nanoscale lithium islands embedded in ionically conductive solid matrix journal April 2017
Designing toughness and strength for soft materials journal July 2017
Electrochemical aspects of the generation of ramified metallic electrodeposits journal December 1990
Complexes of Lithium Imide Salts with Tetraglyme and Their Polyelectrolyte Composite Materials journal January 2004
High Lithium Metal Cycling Efficiency in a Room-Temperature Ionic Liquid journal January 2004
The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces journal January 2005
Fast Charge/Discharge of Li Metal Batteries Using an Ionic Liquid Electrolyte journal January 2013
Correlation between Battery Performance and Lithium Ion Diffusion in Glyme–Lithium Bis(trifluoromethanesulfonyl)amide Equimolar Complexes journal January 2012
Li + Transference Numbers in Liquid Electrolytes Obtained by Very-Low-Frequency Impedance Spectroscopy at Variable Electrode Distances journal January 2016
Solvate Ionic Liquid Electrolyte for Li–S Batteries journal January 2013
Physicochemical Properties of Glyme–Li Salt Complexes as a New Family of Room-temperature Ionic Liquids journal July 2010
Room-Temperature Ionic Liquid-Organic Solvent Mixtures: Conductivity and Ionic Association journal January 2005