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
 

Effects of Imide–Orthoborate Dual-Salt Mixtures in Organic Carbonate Electrolytes on the Stability of Lithium Metal Batteries

Journal Article · · ACS Applied Materials and Interfaces
 [1];  [2];  [3];  [4];  [2];  [2];  [5];  [6];  [2];  [2]
  1. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States; School of Materials Science and Engineering, Southwest Petroleum University, Chengdu, Sichuan 610500, China
  2. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
  3. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
  4. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
  5. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States; State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, China
  6. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States; School of Energy Research, Xiamen University, Xiamen, Fujian 361102, China
+ Show Author Affiliations

The effects of lithium imide and lithium orthoborate dual-salt electrolytes of different salt chemistries in carbonate solvents on the cycling stability of Li metal batteries were systematically and comparatively investigated. Two imide salts (LiTFSI and LiFSI) and two orthoborate salts (LiBOB and LiDFOB) were chosen for this study and compared with the conventional LiPF6 salt. The cycling stability of the Li metal cells with the electrolytes follows the order from good to poor as LiTFSI-LiBOB > LiTFSI-LiDFOB > LiPF6 > LiFSI-LiBOB > LiFSI-LiDFOB, indicating that LiTFSI behaves better than LiFSI and LiBOB over LiDFOB in these four dual-salt mixtures. The LiTFSI-LiBOB can effectively protect the Al substrate and form a more robust surface film on Li metal anode, while the LiFSI-LiBOB results in serious corrosion to the stainless steel cell case and a thicker and looser surface film on Li anode. Computational calculations indicate that the chemical and electrochemical stabilities also follow the order of LiTFSI-LiBOB > LiTFSI-LiDFOB > LiFSI-LiBOB > LiFSI-LiDFOB. The key findings of this work emphasize that the salt chemistry is critically important for enhancing the interfacial stability of Li metal anode and should be carefully manipulated in the development of high performance Li metal batteries.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1434853
Report Number(s):
PNNL-SA-128903; 49321; VT1201000
Journal Information:
ACS Applied Materials and Interfaces, Vol. 10, Issue 3; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

References (37)

Lithium metal anodes for rechargeable batteries January 2014
SiO 2 Hollow Nanosphere-Based Composite Solid Electrolyte for Lithium Metal Batteries to Suppress Lithium Dendrite Growth and Enhance Cycle Life January 2016
Reviving the lithium metal anode for high-energy batteries March 2017
High rate and stable cycling of lithium metal anode February 2015
Research Progress towards Understanding the Unique Interfaces between Concentrated Electrolytes and Electrodes for Energy Storage Applications March 2017
Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism March 2013
Electrolyte additive enabled fast charging and stable cycling lithium metal batteries March 2017
An Artificial Solid Electrolyte Interphase Layer for Stable Lithium Metal Anodes December 2015
Improved Cycle Life and Stability of Lithium Metal Anodes through Ultrathin Atomic Layer Deposition Surface Treatments September 2015
Selective deposition and stable encapsulation of lithium through heterogeneous seeded growth February 2016
Stabilizing Lithium Metal Anodes by Uniform Li-Ion Flux Distribution in Nanochannel Confinement November 2016
Mechanical Surface Modification of Lithium Metal: Towards Improved Li Metal Anode Performance by Directed Li Plating December 2014
Layered reduced graphene oxide with nanoscale interlayer gaps as a stable host for lithium metal anodes March 2016
Highly Stable Operation of Lithium Metal Batteries Enabled by the Formation of a Transient High-Concentration Electrolyte Layer February 2016
A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions June 2002
Failure Mechanism for Fast-Charged Lithium Metal Batteries with Liquid Electrolytes September 2014
Enhanced charging capability of lithium metal batteries based on lithium bis(trifluoromethanesulfonyl)imide-lithium bis(oxalato)borate dual-salt electrolytes June 2016
Mixed salts of LiTFSI and LiBOB for stable LiFePO4-based batteries at elevated temperatures January 2014
A novel dual-salts of LiTFSI and LiODFB in LiFePO4-based batteries for suppressing aluminum corrosion and improving cycling stability November 2015
Dual-salts of LiTFSI and LiODFB for high voltage cathode LiNi0.5Mn1.5O4 July 2016
Mixed Salts of LiFSI and LiODFB for Stable LiCoO 2 -Based Batteries January 2016
The calculation of small molecular interactions by the differences of separate total energies. Some procedures with reduced errors October 1970
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density January 1988
Thermal Reactions of LiPF[sub 6] with Added LiBOB January 2007
Investigation of the Disproportionation Reactions and Equilibrium of Lithium Difluoro(Oxalato) Borate (LiDFOB) January 2011
Effects of cell positive cans and separators on the performance of high-voltage Li-ion batteries September 2012
Effects of Carbonate Solvents and Lithium Salts on Morphology and Coulombic Efficiency of Lithium Electrode January 2013
Analysis of Vinylene Carbonate Derived SEI Layers on Graphite Anode January 2004
Surface chemistry and morphology of the solid electrolyte interphase on silicon nanowire lithium-ion battery anodes April 2009
Behavior of Lithium Metal Anodes under Various Capacity Utilization and High Current Density in Lithium Metal Batteries January 2018
A surface science approach to cathode/electrolyte interfaces in Li-ion batteries: Contact properties, charge transfer and reactions December 2014
Lithium difluoro(oxalato)borate as an additive to suppress the aluminum corrosion in lithium bis(fluorosulfony)imide-based nonaqueous carbonate electrolyte November 2015
Investigation of solid electrolyte interface (SEI) film on LiCoO2 cathode in fluoroethylene carbonate (FEC)-containing electrolyte by 2D correlation X-ray photoelectron spectroscopy (XPS) July 2014
Inhibition of anodic corrosion of aluminum cathode current collector on recharging in lithium imide electrolytes May 2000
Corrosion Prevention Mechanism of Aluminum Metal in Superconcentrated Electrolytes July 2015
Stress corrosion cracking behavior of cold-drawn 316 austenitic stainless steels in simulated PWR environment November 2016
Proton implantation effect on (SUS-316) stainless steel April 2015

Cited By (16)

A dual-salt coupled fluoroethylene carbonate succinonitrile-based electrolyte enables Li-metal batteries January 2020
A self-healing interface on lithium metal with lithium difluoro (bisoxalato) phosphate for enhanced lithium electrochemistry January 2019
Using Triethyl Phosphate to Increase the Solubility of LiNO 3 in Carbonate Electrolytes for Improving the Performance of the Lithium Metal Anode January 2019
Adiponitrile (C 6 H 8 N 2 ): A New Bi‐Functional Additive for High‐Performance Li‐Metal Batteries May 2019
A Dual-Salt Gel Polymer Electrolyte with 3D Cross-Linked Polymer Network for Dendrite-Free Lithium Metal Batteries July 2018
Solvating power series of electrolyte solvents for lithium batteries January 2019
Extending the Service Life of High-Ni Layered Oxides by Tuning the Electrode-Electrolyte Interphase September 2018
Stable cycling of high-voltage lithium metal batteries in ether electrolytes July 2018
Formulierung von Elektrolyten mit gemischten Lithiumsalzen für Lithium‐Batterien December 2019
Formulation of Blended‐Lithium‐Salt Electrolytes for Lithium Batteries December 2019
Nonflammable quasi-solid-state electrolyte for stable lithium-metal batteries January 2019
Effect of Dual‐Salt Concentrated Electrolytes on the Electrochemical Performance of Silicon Nanoparticles January 2020
Concentrated Dual-Salt Electrolyte to Stabilize Li Metal and Increase Cycle Life of Anode Free Li-Metal Batteries January 2019
A functional SrF 2 coated separator enabling a robust and dendrite-free solid electrolyte interphase on a lithium metal anode January 2019
In situ formation of a multicomponent inorganic-rich SEI layer provides a fast charging and high specific energy Li-metal battery January 2019
A LiPO 2 F 2 /LiPF 6 dual-salt electrolyte enabled stable cycling performance of nickel-rich lithium ion batteries January 2020

Similar Records

Related Subjects

Li metal batteries
dual-salt electrolyte
solid electrolyte interphase
cathode electrolyte interphase
Environmental Molecular Sciences Laboratory