A Bilayer Electrolyte Design to Enable High-Areal-Capacity Composite Cathodes in Polymer Electrolytes Based Solid-State Lithium Metal Batteries

Ritu Sahore; Guang Yang; Xi Chelsea Chen; Wan Yu Tsai; Jianlin Li; Nancy J. Dudney; Andrew Westover

doi:10.1021/acsaem.2c00050

A Bilayer Electrolyte Design to Enable High-Areal-Capacity Composite Cathodes in Polymer Electrolytes Based Solid-State Lithium Metal Batteries

Ritu Sahore, Guang Yang, Xi Chelsea Chen, Wan Yu Tsai, Jianlin Li, Nancy J. Dudney, Andrew Westover

Energy Storage & Conversion

Research output: Contribution to journal › Article › peer-review

18 Scopus citations

Abstract

High-areal-capacity cathodes are needed for energy-dense solid-state batteries. Here, we demonstrate a bilayer polymer electrolyte design for cycling 3-6 mAh/cm² NMC811 composite cathodes. The bilayer electrolyte comprises a cross-linked poly(ethylene oxide) (PEO)-based electrolyte layer and a linear-PEO-based electrolyte layer. The former provides dendritic resistance, and the latter provides a seamless interface with the cathode during cycling. Using a single layer of either membrane led to severe shorting or extremely low Coulombic efficiency (CE) in the first cycle. The general concept of a rigid dendrites-inhibiting electrolyte facing Li anode and a softer, cathode-integrated electrolyte that ensures contact with the cathodes during cycling may present a pattern for enabling high-energy-density cathodes.

Original language	English
Pages (from-to)	1409-1413
Number of pages	5
Journal	ACS Applied Energy Materials
Volume	5
Issue number	2
DOIs	https://doi.org/10.1021/acsaem.2c00050
State	Published - Feb 28 2022

Funding

This research is sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL), managed by UT-Battelle, LLC for the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. SEM imaging of cell cross-sections was conducted at the Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility.

Keywords

bilayer design
cross-linked- PEO
integrated interfaces
lithium dendrites
polymer electrolytes
solid-state batteries
thick composite cathodes

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10.1021/acsaem.2c00050

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title = "A Bilayer Electrolyte Design to Enable High-Areal-Capacity Composite Cathodes in Polymer Electrolytes Based Solid-State Lithium Metal Batteries",

abstract = "High-areal-capacity cathodes are needed for energy-dense solid-state batteries. Here, we demonstrate a bilayer polymer electrolyte design for cycling 3-6 mAh/cm2 NMC811 composite cathodes. The bilayer electrolyte comprises a cross-linked poly(ethylene oxide) (PEO)-based electrolyte layer and a linear-PEO-based electrolyte layer. The former provides dendritic resistance, and the latter provides a seamless interface with the cathode during cycling. Using a single layer of either membrane led to severe shorting or extremely low Coulombic efficiency (CE) in the first cycle. The general concept of a rigid dendrites-inhibiting electrolyte facing Li anode and a softer, cathode-integrated electrolyte that ensures contact with the cathodes during cycling may present a pattern for enabling high-energy-density cathodes.",

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author = "Ritu Sahore and Guang Yang and Chen, {Xi Chelsea} and Tsai, {Wan Yu} and Jianlin Li and Dudney, {Nancy J.} and Andrew Westover",

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AU - Sahore, Ritu

AU - Yang, Guang

AU - Chen, Xi Chelsea

AU - Tsai, Wan Yu

AU - Li, Jianlin

AU - Dudney, Nancy J.

AU - Westover, Andrew

PY - 2022/2/28

Y1 - 2022/2/28

N2 - High-areal-capacity cathodes are needed for energy-dense solid-state batteries. Here, we demonstrate a bilayer polymer electrolyte design for cycling 3-6 mAh/cm2 NMC811 composite cathodes. The bilayer electrolyte comprises a cross-linked poly(ethylene oxide) (PEO)-based electrolyte layer and a linear-PEO-based electrolyte layer. The former provides dendritic resistance, and the latter provides a seamless interface with the cathode during cycling. Using a single layer of either membrane led to severe shorting or extremely low Coulombic efficiency (CE) in the first cycle. The general concept of a rigid dendrites-inhibiting electrolyte facing Li anode and a softer, cathode-integrated electrolyte that ensures contact with the cathodes during cycling may present a pattern for enabling high-energy-density cathodes.

AB - High-areal-capacity cathodes are needed for energy-dense solid-state batteries. Here, we demonstrate a bilayer polymer electrolyte design for cycling 3-6 mAh/cm2 NMC811 composite cathodes. The bilayer electrolyte comprises a cross-linked poly(ethylene oxide) (PEO)-based electrolyte layer and a linear-PEO-based electrolyte layer. The former provides dendritic resistance, and the latter provides a seamless interface with the cathode during cycling. Using a single layer of either membrane led to severe shorting or extremely low Coulombic efficiency (CE) in the first cycle. The general concept of a rigid dendrites-inhibiting electrolyte facing Li anode and a softer, cathode-integrated electrolyte that ensures contact with the cathodes during cycling may present a pattern for enabling high-energy-density cathodes.

KW - bilayer design

KW - cross-linked- PEO

KW - integrated interfaces

KW - lithium dendrites

KW - polymer electrolytes

KW - solid-state batteries

KW - thick composite cathodes

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A Bilayer Electrolyte Design to Enable High-Areal-Capacity Composite Cathodes in Polymer Electrolytes Based Solid-State Lithium Metal Batteries

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Keywords

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