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 journalArticlepeer-review

61 Scopus citations


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 languageEnglish
Pages (from-to)1473-1480
Number of pages8
JournalACS Energy Letters
Issue number4
StatePublished - 8 Apr 2022
Externally publishedYes


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