Toward High-Voltage Solid-State Li-Metal Batteries with Double-Layer Polymer Electrolytes

Mikel Arrese-Igor; María Martinez-Ibañez; Ekaterina Pavlenko; Maria Forsyth; Haijin Zhu; Michel Armand; Frédéric Aguesse; Pedro López-Aranguren

doi:10.1021/acsenergylett.2c00488

Toward High-Voltage Solid-State Li-Metal Batteries with Double-Layer Polymer Electrolytes

Mikel Arrese-Igor^*, María Martinez-Ibañez, Ekaterina Pavlenko, Maria Forsyth, Haijin Zhu, Michel Armand, Frédéric Aguesse, Pedro López-Aranguren^*

^*Corresponding author for this work

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

55 Scopus citations

Abstract

Solid polymer electrolyte batteries with a Li-metal anode and high-voltage active materials hold promising prospects to increase the energy density and improve the safety of conventional Li-ion batteries. An adequate choice of the polymers used for the cathode (catholyte) and for the separator (electrolyte) to create a sufficient energy gap and improve the chemical compatibility at both the positive electrode and Li-metal anode is required. The present work highlights the advantages of the double-layer polymer electrolyte approach in cells with a LiNixMnyCozO2 active material, a poly(propylene carbonate) (PPC) catholyte, and a poly(ethylene oxide) (PEO) electrolyte. Replacing PEO in the catholyte with PPC results in a remarkably improved cycling performance. In addition, the higher lithium transference number of electrolytes with single lithium ion conductors leads to a smooth cycling of solid-state batteries. Cells with 1 mAh cm-2 deliver 160 mAh g-1, with a capacity retention above 80% over 80 cycles and a Coulombic efficiency close to 100%.

Original language	English
Pages (from-to)	1473-1480
Number of pages	8
Journal	ACS Energy Letters
Volume	7
Issue number	4
DOIs	https://doi.org/10.1021/acsenergylett.2c00488
State	Published - 8 Apr 2022
Externally published	Yes

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title = "Toward High-Voltage Solid-State Li-Metal Batteries with Double-Layer Polymer Electrolytes",

abstract = "Solid polymer electrolyte batteries with a Li-metal anode and high-voltage active materials hold promising prospects to increase the energy density and improve the safety of conventional Li-ion batteries. An adequate choice of the polymers used for the cathode (catholyte) and for the separator (electrolyte) to create a sufficient energy gap and improve the chemical compatibility at both the positive electrode and Li-metal anode is required. The present work highlights the advantages of the double-layer polymer electrolyte approach in cells with a LiNixMnyCozO2 active material, a poly(propylene carbonate) (PPC) catholyte, and a poly(ethylene oxide) (PEO) electrolyte. Replacing PEO in the catholyte with PPC results in a remarkably improved cycling performance. In addition, the higher lithium transference number of electrolytes with single lithium ion conductors leads to a smooth cycling of solid-state batteries. Cells with 1 mAh cm-2 deliver 160 mAh g-1, with a capacity retention above 80% over 80 cycles and a Coulombic efficiency close to 100%.",

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AU - Arrese-Igor, Mikel

AU - Martinez-Ibañez, María

AU - Pavlenko, Ekaterina

AU - Forsyth, Maria

AU - Zhu, Haijin

AU - Armand, Michel

AU - Aguesse, Frédéric

AU - López-Aranguren, Pedro

PY - 2022/4/8

Y1 - 2022/4/8

N2 - Solid polymer electrolyte batteries with a Li-metal anode and high-voltage active materials hold promising prospects to increase the energy density and improve the safety of conventional Li-ion batteries. An adequate choice of the polymers used for the cathode (catholyte) and for the separator (electrolyte) to create a sufficient energy gap and improve the chemical compatibility at both the positive electrode and Li-metal anode is required. The present work highlights the advantages of the double-layer polymer electrolyte approach in cells with a LiNixMnyCozO2 active material, a poly(propylene carbonate) (PPC) catholyte, and a poly(ethylene oxide) (PEO) electrolyte. Replacing PEO in the catholyte with PPC results in a remarkably improved cycling performance. In addition, the higher lithium transference number of electrolytes with single lithium ion conductors leads to a smooth cycling of solid-state batteries. Cells with 1 mAh cm-2 deliver 160 mAh g-1, with a capacity retention above 80% over 80 cycles and a Coulombic efficiency close to 100%.

AB - Solid polymer electrolyte batteries with a Li-metal anode and high-voltage active materials hold promising prospects to increase the energy density and improve the safety of conventional Li-ion batteries. An adequate choice of the polymers used for the cathode (catholyte) and for the separator (electrolyte) to create a sufficient energy gap and improve the chemical compatibility at both the positive electrode and Li-metal anode is required. The present work highlights the advantages of the double-layer polymer electrolyte approach in cells with a LiNixMnyCozO2 active material, a poly(propylene carbonate) (PPC) catholyte, and a poly(ethylene oxide) (PEO) electrolyte. Replacing PEO in the catholyte with PPC results in a remarkably improved cycling performance. In addition, the higher lithium transference number of electrolytes with single lithium ion conductors leads to a smooth cycling of solid-state batteries. Cells with 1 mAh cm-2 deliver 160 mAh g-1, with a capacity retention above 80% over 80 cycles and a Coulombic efficiency close to 100%.

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JO - ACS Energy Letters

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ER -

Toward High-Voltage Solid-State Li-Metal Batteries with Double-Layer Polymer Electrolytes

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