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Assessing cathode–electrolyte interphases in batteries

Journal Article · · Nature Energy
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  1. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
  2. San Francisco State Univ., CA (United States)
  3. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  4. Idaho National Laboratory (INL), Idaho Falls, ID (United States)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States)
  6. Univ. of Washington, Seattle, WA (United States)
  7. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)
  8. Univ. of California, Irvine, CA (United States)
  9. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  10. Jackson State Univ., Jackson, MS (United States)
  11. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  12. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  13. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  14. New Mexico State Univ., Las Cruces, NM (United States)
  15. Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
  16. Univ. of Chicago, IL (United States)
  17. Brown Univ., Providence, RI (United States)
  18. Univ. of Colorado, Boulder, CO (United States)
  19. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  20. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
+ Show Author Affiliations
The cathode-electrolyte interphase plays a pivotal role in determining the usable capacity and cycling stability of electrochemical cells, yet it is overshadowed by its counterpart, the solid-electrolyte interphase. This is primarily due to the prevalence of side reactions, particularly at low potentials on the negative electrode, especially in state-of-the-art Li-ion batteries where the charge cutoff voltage is limited. However, as the quest for high-energy battery technologies intensifies, there is a pressing need to advance the study of cathode-electrolyte interphase properties. Here, we present a comprehensive approach to analyse the cathode-electrolyte interphase in battery systems. We underscore the importance of employing model cathode materials and coin cell protocols to establish baseline performance. Additionally, we delve into the factors behind the inconsistent and occasionally controversial findings related to the cathode-electrolyte interphase. In conclusion, we also address the challenges and opportunities in characterizing and simulating the cathode-electrolyte interphase, offering potential solutions to enhance its relevance to real-world applications.
Research Organization:
Idaho National Laboratory (INL), Idaho Falls, ID (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
US Department of Energy; USDOE; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office (EE-5); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
AC02-05CH11231; AC02-76SF00515; AC05-00OR22725; AC05-76RL01830; AC07-05ID14517; AC36-08GO28308; AC52-07NA27344; NA0003525
OSTI ID:
2475076
Alternate ID(s):
OSTI ID: 2483440
OSTI ID: 2497903
OSTI ID: 2514407
OSTI ID: 2558136
OSTI ID: 2571518
Report Number(s):
INL/JOU--25-82901-Rev000; MainAdminId:72840; MainId:90551; NREL/JA--5K00-89772; PNNL-SA--200480; UUID:fb988b58-e0ea-49de-9ab9-5cc9b8a0173e; MainAdminId:72840; MainId:90551; UUID:fb988b58-e0ea-49de-9ab9-5cc9b8a0173e
Journal Information:
Nature Energy, Journal Name: Nature Energy Journal Issue: 12 Vol. 9; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (89)

Design of Fire‐Resistant Liquid Electrolyte Formulation for Safe and Long‐Cycled Lithium‐Ion Batteries journal August 2021
Delicately Designed Cyano‐Siloxane as Multifunctional Additive Enabling High Voltage LiNi0.9Co0.05Mn0.05O2/Graphite Full Cell with Long Cycle Life at 50 °C journal May 2023
Review of Recent Development of In Situ/Operando Characterization Techniques for Lithium Battery Research journal May 2019
Interfacial Design for a 4.6 V High‐Voltage Single‐Crystalline LiCoO 2 Cathode journal January 2022
Modeling the Solid Electrolyte Interphase: Machine Learning as a Game Changer? journal January 2022
Electrolyte Engineering Toward High Performance High Nickel (Ni ≥ 80%) Lithium‐Ion Batteries journal December 2023
Understanding the Lithium Sulfur Battery System at Relevant Scales journal August 2015
Ni and Co Segregations on Selective Surface Facets and Rational Design of Layered Lithium Transition-Metal Oxide Cathodes journal February 2016
Extending the Service Life of High-Ni Layered Oxides by Tuning the Electrode-Electrolyte Interphase journal September 2018
Advanced Electrolytes for Fast‐Charging High‐Voltage Lithium‐Ion Batteries in Wide‐Temperature Range journal April 2020
High‐Voltage and High‐Safety Practical Lithium Batteries with Ethylene Carbonate‐Free Electrolyte journal November 2021
Insights into the Crossover Effects in Cells with High‐Nickel Layered Oxide Cathodes and Silicon/Graphite Composite Anodes journal February 2022
Enhanced Electrolyte Transport and Kinetics Mitigate Graphite Exfoliation and Li Plating in Fast‐Charging Li‐Ion Batteries journal December 2022
Designing Electrolytes With Controlled Solvation Structure for Fast‐Charging Lithium‐Ion Batteries journal July 2023
Decoding Electrochemical Processes of Lithium‐Ion Batteries by Classical Molecular Dynamics Simulations journal March 2024
Non‐Flammable Electrolyte Enables High‐Voltage and Wide‐Temperature Lithium‐Ion Batteries with Fast Charging journal January 2023
An Electrolyte with Less Space‐Occupying Diluent at Cathode Inner Helmholtz Plane for Stable 4.6 V Lithium‐Ion Batteries journal December 2023
Modelling Bulk Electrolytes and Electrolyte Interfaces with Atomistic Machine Learning journal January 2021
3,3‐Diethylene Di‐Sulfite (DES) as a High‐Voltage Electrolyte Additive for 4.5 V LiNi0.8Co0.1Mn0.1O2/Graphite Batteries with Enhanced Performances journal February 2021
Suppressing Electrode Crosstalk and Prolonging Cycle Life in High‐Voltage Li Ion Batteries: Pivotal Role of Fluorophosphates in Electrolytes journal May 2022
Thermal Runaway of Lithium‐Ion Batteries Employing Flame‐Retardant Fluorinated Electrolytes journal April 2022
Critical Review on cathode–electrolyte Interphase Toward High-Voltage Cathodes for Li-Ion Batteries journal August 2022
Highly stable Ni-rich layered oxide cathode enabled by a thick protective layer with bio-tissue structure journal January 2020
Optimization of fluorinated orthoformate based electrolytes for practical high-voltage lithium metal batteries journal January 2021
Locking oxygen in lattice: A quantifiable comparison of gas generation in polycrystalline and single crystal Ni-rich cathodes journal May 2022
Simultaneous Single Crystal Growth and Segregation of Ni-Rich Cathode Enabled by Nanoscale Phase Separation for Advanced Lithium-Ion Batteries journal September 2023
Critical Parameters for Evaluating Coin Cells and Pouch Cells of Rechargeable Li-Metal Batteries journal April 2019
Achieving highly reproducible results in graphite-based Li-ion full coin cells journal May 2021
Particle size effects on temperature-dependent performance of LiCoO2 in lithium batteries journal August 2006
Effect of electrolytes on the structure and evolution of the solid electrolyte interphase (SEI) in Li-ion batteries: A molecular dynamics study journal October 2011
Study of triallyl phosphate as an electrolyte additive for high voltage lithium-ion cells journal November 2015
Cathode-Electrolyte Interphase in Lithium Batteries Revealed by Cryogenic Electron Microscopy journal January 2021
Extending the high-voltage operation of Graphite/NCM811 cells by constructing a robust electrode/electrolyte interphase layer journal June 2023
Tailoring electrolyte enables high-voltage Ni-rich NCM cathode against aggressive cathode chemistries for Li-ion batteries journal November 2022
Modified cathode-electrolyte interphase toward high-performance batteries journal December 2022
Cycle-Induced Interfacial Degradation and Transition-Metal Cross-Over in LiNi0.8Mn0.1Co0.1O2–Graphite Cells journal February 2022
Applying Classical, Ab Initio, and Machine-Learning Molecular Dynamics Simulations to the Liquid Electrolyte for Rechargeable Batteries journal May 2022
Insight into SEI Growth in Li-Ion Batteries using Molecular Dynamics and Accelerated Chemical Reactions journal August 2021
Charge Density and Redox Potential of LiNiO2 Using Ab Initio Diffusion Quantum Monte Carlo journal February 2020
Predicting the Ion Desolvation Pathway of Lithium Electrolytes and Their Dependence on Chemistry and Temperature journal May 2022
Best Practices for Operando Battery Experiments: Influences of X-ray Experiment Design on Observed Electrochemical Reactivity journal May 2015
Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights journal October 2015
Toward the Practical Use of Cobalt-Free Lithium-Ion Batteries by an Advanced Ether-Based Electrolyte journal September 2021
Synergistic Effect of Dual-Anion Additives Promotes the Fast Dynamics and High-Voltage Performance of Ni-Rich Lithium-Ion Batteries by Regulating the Electrode/Electrolyte Interface journal August 2022
Coupled Experimental–Theoretical Characterization of a Carbon Electrode in Vanadium Redox Flow Batteries using X-ray Absorption Spectroscopy journal February 2024
Enabling High-Energy-Density Cathode for Lithium–Sulfur Batteries journal June 2018
Resolving Nanoscopic and Mesoscopic Heterogeneity of Fluorinated Species in Battery Solid-Electrolyte Interphases by Cryogenic Electron Microscopy journal March 2020
Electrolyte Regulating toward Stabilization of Cobalt-Free Ultrahigh-Nickel Layered Oxide Cathode in Lithium-Ion Batteries journal March 2021
Beyond Composition: Surface Reactivity and Structural Arrangement of the Cathode–Electrolyte Interphase journal October 2023
Synergistic Degradation Mechanism in Single Crystal Ni-Rich NMC//Graphite Cells journal November 2023
Electrolytes and Interphases in Li-Ion Batteries and Beyond journal October 2014
Unusual Stability of Acetonitrile-Based Superconcentrated Electrolytes for Fast-Charging Lithium-Ion Batteries journal March 2014
Effect of the Electric Double Layer (EDL) in Multicomponent Electrolyte Reduction and Solid Electrolyte Interphase (SEI) Formation in Lithium Batteries journal January 2023
DFT+U Calculations and XAS Study: Further Confirmation of the Presence of CoO 5 Square-Based Pyramids with IS-Co 3+ in Li-Overstoichiometric LiCoO 2 journal December 2013
Metal segregation in hierarchically structured cathode materials for high-energy lithium batteries journal January 2016
State-of-the-art characterization techniques for advanced lithium-ion batteries journal March 2017
Inhibition of transition metals dissolution in cobalt-free cathode with ultrathin robust interphase in concentrated electrolyte journal July 2020
Multifunctional solvent molecule design enables high-voltage Li-ion batteries journal April 2023
Tailoring grain boundary structures and chemistry of Ni-rich layered cathodes for enhanced cycle stability of lithium-ion batteries journal June 2018
Pathways for practical high-energy long-cycling lithium metal batteries journal February 2019
Ultrafast ion transport at a cathode–electrolyte interface and its strong dependence on salt solvation journal June 2020
From laboratory innovations to materials manufacturing for lithium-based batteries journal March 2023
Direct in situ measurements of electrical properties of solid–electrolyte interphase on lithium metal anodes journal September 2023
Electrolyte design for Li-ion batteries under extreme operating conditions journal February 2023
Sensing as the key to battery lifetime and sustainability journal March 2022
Important factors for the reliable and reproducible preparation of non-aqueous electrolyte solutions for lithium batteries journal February 2023
Electrochemical potential window of battery electrolytes: the HOMO–LUMO misconception journal January 2018
Cation-disordered rocksalt transition metal oxides and oxyfluorides for high energy lithium-ion cathodes journal January 2020
Two electrolyte decomposition pathways at nickel-rich cathode surfaces in lithium-ion batteries journal January 2022
A self-purifying electrolyte enables high energy Li ion batteries journal January 2022
High-safety and high-efficiency electrolyte design for 4.6 V-class lithium-ion batteries with a non-solvating flame-retardant journal January 2023
Accurate Electronic Properties and Intercalation Voltages of Olivine-Type Li-Ion Cathode Materials from Extended Hubbard Functionals journal October 2022
Combination of first-principles molecular dynamics and XANES simulations for LiCoO2 -electrolyte interfacial reactions in a lithium-ion battery journal July 2017
Reversible planar gliding and microcracking in a single-crystalline Ni-rich cathode journal December 2020
AC Impedance Analysis of Polycrystalline Insertion Electrodes: Application to Li[sub 1−x]CoO[sub 2] journal January 1985
Formation of Lithium-Graphite Intercalation Compounds in Nonaqueous Electrolytes and Their Application as a Negative Electrode for a Lithium Ion (Shuttlecock) Cell journal January 1993
Studies of the SEI layers in Li(Ni 0.5 Mn 0.3 Co 0.2 )O 2 /Artificial Graphite Cells after Formation and after Cycling journal January 2020
NaH2PO4 as an Electrolyte Additive for Enhanced Thermal Stability of LiNi0.8Co0.1Mn0.1O2/Graphite Batteries journal September 2020
Thermal Runaway Suppression of High-Energy Lithium-Ion Batteries by Designing the Stable Interphase journal September 2021
Perspective—Electrochemistry in Understanding and Designing Electrochemical Energy Storage Systems journal January 2022
To Pave the Way for Large-Scale Electrode Processing of Moisture-Sensitive Ni-Rich Cathodes journal February 2022
Review—Earth-Abundant, Mn-Rich Cathodes for Vehicle Applications and Beyond: Overview of Critical Barriers journal March 2023
Long-Term Cycling and Mechanisms of Cell Degradation of Single Crystal LiNi0.95Mn0.04Co0.01O2/Graphite Cells journal January 2024
Effect of Ambient Storage on the Degradation of Ni-Rich Positive Electrode Materials (NMC811) for Li-Ion Batteries journal January 2018
LiNi 0.4 Mn 1.6 O 4 /Electrolyte and Carbon Black/Electrolyte High Voltage Interfaces: To Evidence the Chemical and Electronic Contributions of the Solvent on the Cathode-Electrolyte Interface Formation journal January 2012
Quantifying Changes to the Electrolyte and Negative Electrode in Aged NMC532/Graphite Lithium-Ion Cells journal January 2018
Studies of the Effect of High Voltage on the Impedance and Cycling Performance of Li[Ni 0.4 Mn 0.4 Co 0.2 ]O 2 /Graphite Lithium-Ion Pouch Cells journal January 2015
Study of the Failure Mechanisms of LiNi 0.8 Mn 0.1 Co 0.1 O 2 Cathode Material for Lithium Ion Batteries journal January 2015
Improving the High Voltage Cycling of Li[Ni 0.42 Mn 0.42 Co 0.16 ]O 2 (NMC442)/Graphite Pouch Cells Using Electrolyte Additives journal January 2014

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25 ENERGY STORAGE
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