Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Stabilizing Graphite Anode in Electrolytes with Nanoscale Anion Networking for High-Rate Lithium Storage

Journal Article · · ACS Energy Letters
 [1];  [2];  [3];  [3];  [3];  [2];  [4];  [5];  [5];  [6];  [2];  [7];  [8];  [2];  [3];  [1]
  1. Purdue Univ., West Lafayette, IN (United States)
  2. Argonne National Laboratory (ANL), Argonne, IL (United States)
  3. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
  5. Northern Illinois Univ., DeKalb, IL (United States)
  6. Indiana University, Indianapolis IN (United States)
  7. Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  8. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
+ Show Author Affiliations
Graphite is the preferred anode material in commercial lithium-ion batteries (LIBs), but its limited compatibility with various organic molecules restricts the electrolyte solvent options. The primary challenge is solvent co-intercalation with Li ions, leading to graphite layer exfoliation. As a result, electrolyte selection often relies on ethylene carbonate (EC)-based solvents. Here, in this study, we introduce electrolytes featuring a nanoscale anion network ordering that hinders the liquid-phase exfoliation of graphite. This network, formed from concentrated long-chain lithium salts, traps free dioxolane (DOL) molecules, reducing the interactions between graphite particles and solvents during Li intercalation. Our findings reveal a mechanism that stabilizes graphite in otherwise unstable solvents with concentrated salts like LiTFSI, providing key insights for improving LIB performance by addressing electrolyte limitations on graphite anodes.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357; AC05-76RL01830; SC0012704
OSTI ID:
2475474
Alternate ID(s):
OSTI ID: 2511209
Report Number(s):
BNL--226276-2024-JAAM; PNNL-SA--203838
Journal Information:
ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 10 Vol. 9; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (55)

The Exfoliation of Graphene in Liquids by Electrochemical, Chemical, and Sonication‐Assisted Techniques: A Nanoscale Study journal April 2013
Exploiting Lithium-Ether Co-Intercalation in Graphite for High-Power Lithium-Ion Batteries journal June 2017
Regulating the Hidden Solvation‐Ion‐Exchange in Concentrated Electrolytes for Stable and Safe Lithium Metal Batteries journal June 2020
Insights into the Nanostructure, Solvation, and Dynamics of Liquid Electrolytes through Small‐Angle X‐Ray Scattering journal December 2020
Ethylene Carbonate‐Free Propylene Carbonate‐Based Electrolytes with Excellent Electrochemical Compatibility for Li‐Ion Batteries through Engineering Electrolyte Solvation Structure journal March 2021
Lithium Nitrate Solvation Chemistry in Carbonate Electrolyte Sustains High-Voltage Lithium Metal Batteries journal September 2018
Lithium Nitrate Regulated Sulfone Electrolytes for Lithium Metal Batteries journal September 2020
Inhibiting Solvent Co‐Intercalation in a Graphite Anode by a Localized High‐Concentration Electrolyte in Fast‐Charging Batteries journal December 2020
Highly Stable Lithium Metal Batteries Enabled by Regulating the Solvation of Lithium Ions in Nonaqueous Electrolytes journal March 2018
Intercalation of lithium into graphite and other carbons journal August 1975
A reversible graphite-lithium negative electrode for electrochemical generators journal January 1983
Recent studies on the correlation between surface chemistry, morphology, three-dimensional structures and performance of Li and Li-C intercalation anodes in several important electrolyte systems journal September 1997
Insight into the nanostructure of “water in salt” solutions: A SAXS/WAXS study on imide-based lithium salts aqueous solutions journal March 2022
Fluorinated Solid-Electrolyte Interphase in High-Voltage Lithium Metal Batteries journal November 2019
New insights into pre-lithiation kinetics of graphite anodes via nuclear magnetic resonance spectroscopy journal February 2018
The reactivity of charged positive Li1-n[NixMnyCoz]O2 electrodes with electrolyte at elevated temperatures using accelerating rate calorimetry journal June 2018
Temperature dependent electrochemical performance of graphite anodes for K-ion and Li-ion batteries journal January 2019
A stable graphite electrode in superconcentrated LiTFSI-DME/DOL electrolyte and its application in lithium-sulfur full battery journal November 2017
Observed bands in Raman and infrared spectra of 1,3-dioxolane and their assignments journal January 2013
Revealing the Correlation between the Solvation Structures and the Transport Properties of Water-in-Salt Electrolytes journal February 2023
Relationship of the Molecular Structure and Transport Properties of Imide-Based Lithium Salts of “Acetonitrile/Water-in-Salt” Electrolytes journal August 2023
Unveiling the Liquid Electrolyte Solvation Structure by Small Angle X-ray Scattering journal December 2023
Formation of Reversible Solid Electrolyte Interface on Graphite Surface from Concentrated Electrolytes journal February 2017
Building Better Li Metal Anodes in Liquid Electrolyte: Challenges and Progress journal December 2020
New Insights on Graphite Anode Stability in Rechargeable Batteries: Li Ion Coordination Structures Prevail over Solid Electrolyte Interphases journal January 2018
Mechanisms of Liquid-Phase Exfoliation for the Production of Graphene journal June 2020
Solvation Structure of Methanol-in-Salt Electrolyte Revealed by Small-Angle X-ray Scattering and Simulations journal February 2024
General Observation of Lithium Intercalation into Graphite in Ethylene-Carbonate-Free Superconcentrated Electrolytes journal March 2014
Liquid Exfoliation of Defect-Free Graphene journal March 2012
Unusual Stability of Acetonitrile-Based Superconcentrated Electrolytes for Fast-Charging Lithium-Ion Batteries journal March 2014
Solvate Structures and Spectroscopic Characterization of LiTFSI Electrolytes journal September 2014
Mechanism of Li Ion Desolvation at the Interface of Graphite Electrode and Glyme–Li Salt Solvate Ionic Liquids journal August 2014
Magnetically aligned graphite electrodes for high-rate performance Li-ion batteries journal July 2016
Stable lithium electrodeposition in liquid and nanoporous solid electrolytes journal August 2014
High-yield production of graphene by liquid-phase exfoliation of graphite journal August 2008
Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode journal September 2018
Overlooked electrolyte destabilization by manganese (II) in lithium-ion batteries journal July 2019
Non-flammable electrolytes with high salt-to-solvent ratios for Li-ion and Li-metal batteries journal July 2018
Localized high-concentration electrolytes get more localized through micelle-like structures journal November 2023
Non-flammable electrolyte enables Li-metal batteries with aggressive cathode chemistries journal July 2018
Fragmentation and exfoliation of 2-dimensional materials: a statistical approach journal January 2014
A comparative study of graphite electrodes using the co-intercalation phenomenon for rechargeable Li, Na and K batteries journal January 2016
Intercalation chemistry of graphite: alkali metal ions and beyond journal January 2019
A review on energy chemistry of fast-charging anodes journal January 2020
The success story of graphite as a lithium-ion anode material – fundamentals, remaining challenges, and recent developments including silicon (oxide) composites journal January 2020
Electrolyte design implications of ion-pairing in low-temperature Li metal batteries journal January 2022
Kinetic pathways of fast lithium transport in solid electrolyte interphases with discrete inorganic components journal January 2023
From graphite to graphene: direct liquid-phase exfoliation of graphite to produce single- and few-layered pristine graphene journal January 2013
Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries journal January 2018
Solvent screening for efficient chemical exfoliation of graphite journal November 2020
Phase diagram of Li x C 6 journal November 1991
Correlation Between Cointercalation of Solvents and Electrochemical Intercalation of Lithium into Graphite in Propylene Carbonate Solution journal January 2003
The Electrochemical Decomposition of Propylene Carbonate on Graphite journal January 1970
Mechanism of Gases Generation during Lithium-Ion Batteries Cycling journal January 2019
Reversible Capacity of Conductive Carbon Additives at Low Potentials: Caveats for Testing Alternative Anode Materials for Li-Ion Batteries journal December 2016

Similar Records

Design Criteria of Dilute Ether Electrolytes toward Reversible and Fast Intercalation Chemistry of Graphite Anode in Li-Ion Batteries
Journal Article · Mon Feb 13 00:00:00 UTC 2023 · ACS Energy Letters · OSTI ID:1960520

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY