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

doi:10.1021/acsami.0c17422

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

ACS Appl Mater Interfaces. 2021 Jan 20;13(2):2507-2520. doi: 10.1021/acsami.0c17422. Epub 2021 Jan 6.

Authors

Kumlachew Zelalem Walle¹, Lakshmipriya Musuvadhi Babulal¹, She Huang Wu², Wen-Chen Chien^{1

3}, Rajan Jose⁴, Shingjiang Jessie Lue^{5

6

7}, Jeng-Kuei Chang⁸, Chun-Chen Yang^{1

3

5}

Affiliations

¹ Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 24301, Taiwan, R.O.C.
² Graduate Institute of Science and Technology, National Taiwan University of Science and Technology, 43, Sec. 4, Keelung Road, Taipei 106, Taiwan, R.O.C.
³ Department of Chemical Engineering, Ming Chi University of Technology, New Taipei City 24301, Taiwan, R.O.C.
⁴ Nanostructured Renewable Energy Materials Laboratory, Faculty of Industrial Sciences and Technology, University Malaysia Pahang, 26300 Kuantan, Malaysia.
⁵ Department of Chemical and Materials Engineering, and Green Technology Research Center, Chang Gung University, Taoyuan City 333, Taiwan, R.O.C.
⁶ Department of Radiation Oncology, Chang Gung Memorial Hospital, Taoyuan City 333, Taiwan, R.O.C.
⁷ Department of Safety, Health and Environmental Engineering, Ming Chi University of Technology, New Taipei City 243, Taiwan, R.O.C.
⁸ Department of Materials Science and Engineering, National Chiao Tung University, Hsinchu, 30010, Taiwan, R.O.C.

PMID: 33406841
DOI: 10.1021/acsami.0c17422

Abstract

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 Ni_0.8Co_0.1Mn_0.1O₂ (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.

Keywords: Ga/F-LLZO; Li/Nafion; Taylor flow reactor; composite polymer electrolyte; nickel-rich NCM811 cathode.