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

Title: Comparing measurement of limiting current in block copolymer electrolytes as a function of salt concentration with theoretical predictions

Journal Article · · Electrochimica Acta
 [1];  [2];  [1];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States)

Optimizing electrolyte performance is crucial for the widespread adoption of electrochemical energy storage. We demonstrate that limiting current provides a robust criterion for determining the optimum electrolyte. Experiments were conducted on rigid block copolymer electrolytes comprising mixtures of polystyrene-block-poly(ethylene oxide) copolymer (SEO) and lithium bis(trifluoromethanesulfonyl) imide salt (LiTFSI) over a salt concentration range from rav = 0.04 to rav = 0.20 (rav is the molar ratio of lithium ions to ethylene oxide). Here we show that the maximum limiting current density is 4.3 mA cm–2 at rav = 0.12. The dependence of limiting current on salt concentration is in good agreement with predictions from Newman's concentrated solution theory with no adjustable parameters.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1958526
Journal Information:
Electrochimica Acta, Journal Name: Electrochimica Acta Vol. 409; ISSN 0013-4686
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (41)

Butyllithium-Initiated Anionic Synthesis of Well-Defined Poly(styrene-block-ethylene oxide) Block Copolymers with Potassium Salt Additives journal January 1996
Recent Progress of the Solid-State Electrolytes for High-Energy Metal-Based Batteries journal January 2018
A study of electrochemical kinetics of lithium ion in organic electrolytes journal July 2002
Electrochemical measurement of transference numbers in polymer electrolytes journal December 1987
Estimation of Li+ transport number in polymer electrolytes by the combination of complex impedance and potentiostatic polarization measurements journal September 1988
Conductivity and transference number measurements on polymer electrolytes journal September 1988
A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions journal June 2002
Review of selected electrode–solution interactions which determine the performance of Li and Li ion batteries journal August 2000
Electrochemical studies of ferrocene in a lithium ion conducting organic carbonate electrolyte journal November 2009
A solid-state single-ion polymer electrolyte with ultrahigh ionic conductivity for dendrite-free lithium metal batteries journal May 2019
Limiting current density in bis(trifluoromethylsulfonyl)amide-based ionic liquid for lithium batteries journal February 2011
Lithium-ion batteries – Current state of the art and anticipated developments journal December 2020
Diffusion and migration in polymer electrolytes journal April 2020
Effect of salt concentration profiles on protrusion growth in lithium-polymer‑lithium cells journal December 2020
Special Editorial Perspective: Beyond Li-Ion Battery Chemistry journal July 2020
Growth of Lithium Dendrites and Globules through a Solid Block Copolymer Electrolyte as a Function of Current Density journal November 2018
Comparing Measurements of Limiting Current of Electrolytes with Theoretical Predictions up to the Solubility Limit journal September 2019
Limiting Current in Nanostructured Block Copolymer Electrolytes journal April 2021
Impact of Salt Concentration on Nonuniform Lithium Electrodeposition through Rigid Block Copolymer Electrolytes journal November 2019
Battery Separators journal October 2004
Polymers with Complex Architecture by Living Anionic Polymerization journal December 2001
The Limiting Current on a Rotating Disc Electrode in Potassium Iodide-Potassium Triiodide Solutions journal March 1954
Effect of Molecular Weight on the Mechanical and Electrical Properties of Block Copolymer Electrolytes journal June 2007
Ionic Conductivity of Low Molecular Weight Block Copolymer Electrolytes journal January 2013
Single-ion BAB triblock copolymers as highly efficient electrolytes for lithium-metal batteries journal March 2013
Detection of subsurface structures underneath dendrites formed on cycled lithium metal electrodes journal November 2013
Ohm’s law for ion conduction in lithium and beyond-lithium battery electrolytes journal July 2019
Energy storage emerging: A perspective from the Joint Center for Energy Storage Research journal June 2020
On the Concentration at the Electrodes in a Solution, with special reference to the Liberation of Hydrogen by Electrolysis of a Mixture of Copper Sulphate and Sulphuric Acid journal October 1899
Dendrite Growth in Lithium/Polymer Systems journal January 2003
Fiftieth Anniversary: Diffusion and Convection in Electrolysis—A Theoretical Review journal January 1952
Resolution of the Modulus versus Adhesion Dilemma in Solid Polymer Electrolytes for Rechargeable Lithium Metal Batteries journal January 2012
Electrochemical Deposition and Stripping Behavior of Lithium Metal across a Rigid Block Copolymer Electrolyte Membrane journal January 2015
Comparing Experimental Measurements of Limiting Current in Polymer Electrolytes with Theoretical Predictions journal January 2019
Negative Stefan-Maxwell Diffusion Coefficients and Complete Electrochemical Transport Characterization of Homopolymer and Block Copolymer Electrolytes journal January 2018
Relationship between Steady-State Current in Symmetric Cells and Transference Number of Electrolytes Comprising Univalent and Multivalent Ions journal January 2015
Failure Mode of Lithium Metal Batteries with a Block Copolymer Electrolyte Analyzed by X-Ray Microtomography journal January 2015
Comparing Cycling Characteristics of Symmetric Lithium-Polymer-Lithium Cells with Theoretical Predictions journal January 2018
Polymer and composite electrolytes journal October 2018
Factors That Control the Formation of Dendrites and Other Morphologies on Lithium Metal Anodes journal November 2019
Lithium Dendrite Formation on a Lithium Metal Anode from Liquid, Polymer and Solid Electrolytes journal January 2016