Correlation between Redox Potential and Solvation Structure in Biphasic Electrolytes for Li Metal Batteries (Journal Article) (2024)

Journal Article · · Advanced Science

Park, Kyobin[1]; Kim, Dong‐Min[2]; Ha, Kwang‐Ho[1]; Kwon, Bomee[1]; Lee, Jeonghyeop[1]; Jo, Seunghyeon[1]; Ji, Xiulei[3]; Lee, Kyu Tae Correlation between Redox Potential and Solvation Structure in Biphasic Electrolytes for Li Metal Batteries (Journal Article) (1)[1]

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  1. School of Chemical and Biological Engineering Institute of Chemical Processes Seoul National University 1 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of Korea
  2. The Molecular Foundry and the Joint Center for Energy Storage Research Department Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
  3. Department of Chemistry Oregon State University Corvallis OR 97331‐4003 USA

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Abstract The activity of lithium ions in electrolytes depends on their solvation structures. However, the understanding of changes in Li+activity is still elusive in terms of interactions between lithium ions and solvent molecules. Herein, the chelating effect of lithium ion by forming [Li(15C5)]+gives rise to a decrease in Li+activity, leading to the negative potential shift of Li metal anode. Moreover, weakly solvating lithium ions in ionic liquids, such as [Li(TFSI)2](TFSI = bis(trifluoromethanesulfonyl)imide),increase in Li+activity, resulting in the positive potential shift of LiFePO4cathode. This allows the development of innovative high energy density Li metal batteries, such as 3.8V class Li | LiFePO4cells, along with introducing stable biphasic electrolytes. In addition, correlation between Li+activity, cell potential shift, and Li+solvation structure is investigated by comparing solvated Li+ions with carbonate solvents, chelated Li+ions with cyclic and linear ethers, and weakly solvating Li+ions in ionic liquids. These findings elucidate a broader understanding of the complex origin of Li+activity and provide an opportunity to achieve high energy density lithium metal batteries.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2470265
Journal Information:
Advanced Science, Vol. 9, Issue 33; ISSN 2198-3844
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (46)

Electrolytes and Interphases in Li-Ion Batteries and Beyond journal October 2014
Challenges and opportunities towards fast-charging battery materials journal June 2019
Critical effects of electrolyte recipes for Li and Na metal batteries journal September 2021
Achieving three-dimensional lithium sulfide growth in lithium-sulfur batteries using high-donor-number anions journal January 2019
An Electron/Ion Dual‐Conductive Alloy Framework for High‐Rate and High‐Capacity Solid‐State Lithium‐Metal Batteries journal September 2018
High-voltage positive electrode materials for lithium-ion batteries journal January 2017
Polycrystalline and Single Crystalline NCM Cathode Materials—Quantifying Particle Cracking, Active Surface Area, and Lithium Diffusion journal March 2021
High‐Energy Ni‐Rich Cathode Materials for Long‐Range and Long‐Life Electric Vehicles journal April 2022
Hydrophobic Ni-Rich Layered Oxides as Cathode Materials for Lithium-Ion Batteries journal August 2019
Quantifying inactive lithium in lithium metal batteries journal August 2019
Design principles for electrolytes and interfaces for stable lithium-metal batteries journal September 2016
Lithium metal anodes for rechargeable batteries journal January 2014
A cooperative biphasic MoOx–MoPx promoter enables a fast-charging lithium-ion battery journal January 2021
Polymer Interface-Dependent Morphological Transition toward Two-Dimensional Porous Inorganic Nanocoins as an Ultrathin Multifunctional Layer for Stable Lithium–Sulfur Batteries journal September 2021
Fluorinated co-solvent promises Li-S batteries under lean-electrolyte conditions journal November 2020
Promise and reality of post-lithium-ion batteries with high energy densities journal March 2016
Advanced Hybrid Electrolyte Li-O2 Battery Realized by Dual Superlyophobic Membrane journal December 2019
"Water-in-salt" electrolyte enables high-voltage aqueous lithium-ion chemistries journal November 2015
Reverse Dual-Ion Battery via a ZnCl 2 Water-in-Salt Electrolyte journal March 2019
Hydrate-melt electrolytes for high-energy-density aqueous batteries journal August 2016
Molecular crowding electrolytes for high-voltage aqueous batteries journal April 2020
Polysulfide-based redox flow batteries with long life and low levelized cost enabled by charge-reinforced ion-selective membranes journal April 2021
New Concepts in Electrolytes journal February 2020
Predicting the Ion Desolvation Pathway of Lithium Electrolytes and Their Dependence on Chemistry and Temperature journal May 2022
Complex Growth Behavior of Li Dendrites in Al2O3 Nanoparticles‐Driven Viscoelastic Electrolytes for Lithium Metal Batteries: Dynamic versus Quasistatic Rheology journal July 2021
Potentiometric Measurement to Probe Solvation Energy and Its Correlation to Lithium Battery Cyclability journal June 2021
Localized High-Concentration Sulfone Electrolytes for High-Efficiency Lithium-Metal Batteries journal August 2018
Mechanism of Li Ion Desolvation at the Interface of Graphite Electrode and Glyme–Li Salt Solvate Ionic Liquids journal August 2014
Crown Ethers as Electrolyte Additives To Modulate the Electrochemical Potential of Lithium Organic Batteries journal August 2019
Monolithic heterojunction quasi-solid-state battery electrolytes based on thermodynamically immiscible dual phases journal January 2019
Double-Layer Polymer Electrolyte for High-Voltage All-Solid-State Rechargeable Batteries journal December 2018
Biphasic Electrolyte Inhibiting the Shuttle Effect of Redox Molecules in Lithium‐Metal Batteries journal June 2021
Design of a Dual-Electrolyte Battery System Based on a High-Energy NCM811-Si/C Full Battery Electrode-Compatible Electrolyte journal November 2021
A dual-electrolyte system for highly efficient Al–air batteries journal January 2022
Thermodynamics of electrolytes. I. Theoretical basis and general equations journal January 1973
Measuring the Salt Activity Coefficient in Lithium-Battery Electrolytes journal January 2008
Electrolytes Enriched by Crown Ethers for Lithium Metal Batteries journal July 2020
Electrochemically Regulated Li Deposition by Crown Ether journal March 2021
Correlating Li-Ion Solvation Structures and Electrode Potential Temperature Coefficients journal January 2021
Macrocyclic effect on the stability of copper(II) tetramine complexes journal November 1969
Thermodynamic origin of the macrocyclic effect in crown ether complexes of sodium(1+), potassium(1+), and barium(2+) journal April 1982
Lithium ion solvation by ethylene carbonates in lithium-ion battery electrolytes, revisited by density functional theory with the hybrid solvation model and free energy correction in solution journal January 2016
FTIR Spectroscopy of Ion Solvation of LiClO4 and LiSCN in Acetonitrile, Benzonitrile, and Propylene Carbonate journal January 2000
Solvation behavior of carbonate-based electrolytes in sodium ion batteries journal January 2017
Regulating Interfacial Chemistry in Lithium‐Ion Batteries by a Weakly Solvating Electrolyte** journal November 2020
Spectroscopic characterization of the conformational states of the bis(trifluoromethanesulfonyl)imide anion (TFSI−) journal January 2005

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Correlation between Redox Potential and Solvation Structure in Biphasic Electrolytes for Li Metal Batteries (Journal Article) (2024)
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