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In Situ Lithiated Reference Electrode: Four Electrode Design for In-operando Impedance Spectroscopy

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Interfacial Design for a 4.6 V High-Voltage Single-Crystalline LiCoO₂ Cathode.

Jiaxun Zhang¹, Peng-Fei Wang¹, Panxing Bai¹

¹Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, 20742, USA.

Advanced Materials (Deerfield Beach, Fla.)

|December 8, 2021

Summary

Single-crystalline lithium cobalt oxide cathodes show improved stability at high voltages. A robust cathode electrolyte interphase (CEI) in a fluorinated electrolyte prevents degradation, enhancing performance for high-energy-density batteries.

Keywords:

high-voltage LiCoO 2 cathodes inorganic-rich cathode electrolyte interphase nonflammable electrolytes single-crystalline cathodes

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Growth and Electrostatic/chemical Properties of Metal/LaAlO3/SrTiO3 Heterostructures

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Published on: February 8, 2018

Area of Science:

Materials Science
Electrochemistry
Battery Technology

Background:

Single-crystalline cathode materials offer superior capacity retention over polycrystalline ones by minimizing surface area and phase boundaries.
Single-crystalline LiCoO2 cathodes face challenges like structural instability and capacity fade at high voltages (4.6 V) due to cobalt dissolution, oxygen loss, and electrolyte penetration.

Purpose of the Study:

To investigate methods for enhancing the structural stability and performance of single-crystalline LiCoO2 cathodes at high operating voltages.
To explore the role of a robust cathode electrolyte interphase (CEI) in mitigating degradation mechanisms.

Main Methods:

Formation of a robust cathode electrolyte interphase (CEI) using an all-fluorinated electrolyte.
Electrochemical testing of single-crystalline LiCoO2 cathodes at high voltage (4.6 V).
Analysis of degradation mechanisms and protective effects of the CEI.

Main Results:

A robust CEI effectively prevents cobalt dissolution and electrolyte penetration, safeguarding the single-crystalline LiCoO2 structure.
Reversible planar gliding along the (003) plane was protected, maintaining structural integrity.
The CEI significantly mitigates performance fading at a high operating voltage of 4.6 V.

Conclusions:

A robust CEI in an all-fluorinated electrolyte is crucial for stabilizing single-crystalline LiCoO2 cathodes at high voltages.
This approach provides a pathway for designing advanced electrolytes to improve the performance of high-energy-density battery materials.
The findings offer new insights into protecting cathode materials from degradation during high-voltage operation.