Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability

Journal Article · · Advanced Energy Materials
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. Univ. of California San Diego, La Jolla, CA (United States)
+ Show Author Affiliations

Calendar aging of lithium metal batteries, in which cells’ components degrade internally due to chemical reactions while no current is being applied, is a relatively unstudied field. In this work, a model to predict calendar aging of lithium metal cells is developed using two sets of readily obtainable data: solid electrolyte interphase (SEI) layer composition (measured via X-ray photoelectron spectroscopy) and SEI stability (measured as a degradation rate using a simple constant current–constant voltage charging protocol). Electrolyte properties such as volume and salt concentration are varied in order to determine their effect on SEI stability and composition, with subsequent impacts to calendar aging. Lower salt concentrations produce a solvent-based, more soluble SEI, while the highest concentration produces a salt-based, less soluble SEI. Higher electrolyte volumes promote dissolution of the SEI and thus decrease its stability. The model predicts that lithium metal would be the limiting factor in calendar aging, depleting long before the electrolyte does. Furthermore, the relative composition of the electrolyte during aging is modeled and found to eventually converge to the same value independent of initial salt concentration.

Research Organization:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
AC07-05ID14517
OSTI ID:
1473703
Report Number(s):
INL/JOU-18-45118-Rev001
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 26 Vol. 8; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (35)

Anode-Free Rechargeable Lithium Metal Batteries journal August 2016
Addressing Passivation in Lithium-Sulfur Battery Under Lean Electrolyte Condition journal February 2018
A Review of Solid Electrolyte Interphases on Lithium Metal Anode journal November 2015
Research Progress towards Understanding the Unique Interfaces between Concentrated Electrolytes and Electrodes for Energy Storage Applications journal March 2017
Failure Mechanism for Fast-Charged Lithium Metal Batteries with Liquid Electrolytes journal September 2014
Highly Stable Operation of Lithium Metal Batteries Enabled by the Formation of a Transient High-Concentration Electrolyte Layer journal February 2016
Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries journal October 2017
Review of selected electrode–solution interactions which determine the performance of Li and Li ion batteries journal August 2000
X-ray photoelectron spectroscopy of negative electrodes from high-power lithium-ion cells showing various levels of power fade journal November 2004
Role of Mixed Solvation and Ion Pairing in the Solution Structure of Lithium Ion Battery Electrolytes journal June 2015
Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal journal January 2017
Problem, Status, and Possible Solutions for Lithium Metal Anode of Rechargeable Batteries journal February 2018
Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy journal October 2016
K + Reduces Lithium Dendrite Growth by Forming a Thin, Less-Resistive Solid Electrolyte Interphase journal July 2016
Role of Solution Structure in Solid Electrolyte Interphase Formation on Graphite with LiPF 6 in Propylene Carbonate journal November 2013
Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes from First-Principles and Classical Reactive Molecular Dynamics journal January 2015
X-ray Photoelectron Spectroscopy Studies of Lithium Surfaces Prepared in Several Important Electrolyte Solutions. A Comparison with Previous Studies by Fourier Transform Infrared Spectroscopy journal January 1996
Superconcentrated electrolytes for a high-voltage lithium-ion battery journal June 2016
A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries journal February 2013
High rate and stable cycling of lithium metal anode journal February 2015
Status and challenges in enabling the lithium metal electrode for high-energy and low-cost rechargeable batteries journal December 2017
A comparative XPS surface study of Li 2 FeSiO 4 /C cycled with LiTFSI- and LiPF 6 -based electrolytes journal January 2009
A novel and accurate analytical method based on X-ray photoelectron spectroscopy for the quantitative detection of the lithium content in LiFePO 4 journal January 2014
Dead lithium: mass transport effects on voltage, capacity, and failure of lithium metal anodes journal January 2017
Electrochemical and Infrared Studies of the Reduction of Organic Carbonates journal January 2001
A Comparative Study of Synthetic Graphite and Li Electrodes in Electrolyte Solutions Based on Ethylene Carbonate-Dimethyl Carbonate Mixtures journal January 1996
The Effect of Vinylene Carbonate Additive on Surface Film Formation on Both Electrodes in Li-Ion Batteries journal January 2009
Effect of Vinylene Carbonate and Fluoroethylene Carbonate on SEI Formation on Graphitic Anodes in Li-Ion Batteries journal January 2015
Investigation of the Lithium Solid Electrolyte Interphase in Vinylene Carbonate Electrolytes Using Cu||LiFePO 4 Cells journal January 2017
Calendar Aging of Lithium-Ion Batteries: I. Impact of the Graphite Anode on Capacity Fade journal January 2016
Highly Quantitative Electrochemical Characterization of Non-Aqueous Electrolytes and Solid Electrolyte Interphases journal December 2013
Reduction Reactions of Electrolyte Salts for Lithium Ion Batteries: LiPF 6 , LiBF 4 , LiDFOB, LiBOB, and LiTFSI journal January 2018
High Rate and Stable Cycling of Lithium Metal Anode journal April 2015
X-ray photoelectron spectroscopy for sulfide glass electrolytes in the systems Li2S–P2S5 and Li2S–P2S5–LiBr journal January 2016
Excitation Energy Dependence for the Li 1s X-ray Photoelectron Spectra of LiMn2O4 journal January 2005

Cited By (3)

Correlation between Li Plating Behavior and Surface Characteristics of Carbon Matrix toward Stable Li Metal Anodes journal November 2018
Room‐Temperature Rechargeable Ca‐Ion Based Hybrid Batteries with High Rate Capability and Long‐Term Cycling Life journal June 2019
On the Reliability of Sodium Metal Anodes: The Influence of Neglected Parameters journal January 2019

Similar Records

Related Subjects

25 ENERGY STORAGE
electrolyte salt concentration
electrolyte volume
lithium metal calendar life
rechargeable lithium batteries
solid electrolyte interphase (SEI) layer stability