• 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 Nanostructured Renewable Energy Materials Laboratory, Faculty of Industrial Sciences and Technology, University Malaysia Pahang, 26300 Kuantan, Malaysia
  • 4 Department of Chemical and Materials Engineering, and Green Technology Research Center, Chang Gung University, Taoyuan City 333, Taiwan, R.O.C
  • 5 Department of Materials Science and Engineering, National Chiao Tung University, Hsinchu, 30010, Taiwan, R.O.C
ACS Appl Mater Interfaces, 2021 Jan 20;13(2):2507-2520.
PMID: 33406841 DOI: 10.1021/acsami.0c17422


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.

* Title and MeSH Headings from MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine.