Electrochemical Characteristics of a Polymer/Garnet Trilayer Composite Electrolyte for Solid-State Lithium-Metal Batteries

Kumlachew Zelalem Walle, Lakshmipriya Musuvadhi Babulal, She Huang Wu, Wen Chen Chien, Rajan Jose, Shingjiang Jessie Lue, Jeng-Kuei Chang, Chun Chen Yang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

25 Scopus citations


Although solid-state Li-metal batteries (LMBs) featuring polymer-based solid electrolytes might one day replace conventional Li-ion batteries, the poor Li-ion conductivity of solid polymer electrolytes at low temperatures has hindered their practical applications. Herein, we describe the first example of using a co-precipitation method in a Taylor flow reactor to produce the metal hydroxides of both the Ga/F dual-doped Li7La3Zr2O12 (Ga/F-LLZO) ceramic electrolyte precursors and the Li2MoO4-modified Ni0.8Co0.1Mn0.1O2 (LMO@T-LNCM 811) cathode materials for LMBs. The Li/Nafion (LiNf)-coated Ga/F-LLZO (LiNf@Ga/F-LLZO) ceramic filler was finely dispersed in the poly(vinylidene fluoride)/polyacrylonitrile/lithium bis(trifluoromethanesulfonimide)/succinonitrile matrix to give a trilayer composite polymer electrolyte (denoted "Tri-CPE") through a simple solution-casting. The bulk ionic conductivity of the Tri-CPE at room temperature was approximately 4.50 × 10-4 S cm-1 and exhibited a high Li+ ion transference number (0.84). It also exhibits a broader electrochemical window of 1-5.04 V versus Li/Li+. A full cell based on a CR2032 coin cell containing the LMO@T-LNCM811-based composite cathode, when cycled under 1 C/1 C at room temperature for 300 cycles, achieved an average Columbic efficiency of 99.4% and a capacity retention of 89.8%. This novel fabrication strategy for Tri-CPE structures has potential applications in the preparation of highly safe high-voltage cathodes for solid-state LMBs.

Original languageEnglish
Pages (from-to)2507-2520
Number of pages14
JournalACS Applied Materials and Interfaces
Issue number2
StatePublished - 20 Jan 2021


  • Ga/F-LLZO
  • Li/Nafion
  • Taylor flow reactor
  • composite polymer electrolyte
  • nickel-rich NCM811 cathode


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