Composite electrolytes engineered by anion acceptors for boosted high-voltage solid-state lithium metal batteries

Jiahui Yu; Kangsheng Huang; Hai Xu; Chang Fang; Xiaogang Zhang

doi:10.1016/j.jcis.2023.03.110

Composite electrolytes engineered by anion acceptors for boosted high-voltage solid-state lithium metal batteries

J Colloid Interface Sci. 2023 Jul 15:642:330-339. doi: 10.1016/j.jcis.2023.03.110. Epub 2023 Mar 21.

Authors

Jiahui Yu¹, Kangsheng Huang¹, Hai Xu², Chang Fang², Xiaogang Zhang³

Affiliations

¹ Jiangsu Key Laboratory of Electrochemical Energy-Storage Technologies, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China; Shenzhen Research Institute, Nanjing University of Aeronautics and Astronautics, Shenzhen 518000, China.
² Jiangsu Key Laboratory of Electrochemical Energy-Storage Technologies, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
³ Jiangsu Key Laboratory of Electrochemical Energy-Storage Technologies, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China; Shenzhen Research Institute, Nanjing University of Aeronautics and Astronautics, Shenzhen 518000, China; Key Laboratory for Intelligent Nano Materials and Devices of the Ministry of Education. Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China. Electronic address: azhangxg@nuaa.edu.cn.

PMID: 37011451
DOI: 10.1016/j.jcis.2023.03.110

Abstract

Solid-state batteries (SSBs) are considered as the most promising option to replace commercial lithium-ion batteries due to their ability to address the flammability of liquid organic electrolytes and facilitate the energy density of lithium batteries. Herein, by introducing tris(trimethylsilyl) borate (TMSB) as anion acceptors, we successfully develop the light and thin electrolyte (TMSB-PVDF-HFP-LLZTO-LiTFSI, PLFB) with a wide voltage window to couple the lithium metal anode with the high-voltage cathodes. Consequently, as-prepared PLFB can greatly boost the generation of free Li⁺ and improve the Li⁺ transference numbers (t_Li+=0.92) at room temperature. Moreover, combined with theoretical calculation and experimental results, the changes in the composition and properties of the composite electrolyte membrane with the addition of anionic receptors are systematically studied, which further implies the intrinsic mechanism of the stability difference. In addition, the PLFB-based SSB assembled by LiNi_0.8Co_0.1Mn_0.1O₂ cathode and lithium anode exhibits a high capacity retention of 86% after loop 400 cycles. This investigation on boosted battery performance by immobilized anions not only contributes to the directional construction of dendrite-free and lithium-ion permeable interface, but also brings new opportunities for the screening and design of the next generation of high-energy SSBs.

Keywords: Anion receptor; Dendrite-free interface; High Li(+) transference number; High ionic conductivity; Solid-state batteries.