Polyether sulfone and Li6.4La3Zr1.4Ta0.6O12 based polymer-in-ceramic electrolyte with enhanced conductivity at low temperature for solid state lithium batteries. (June 2022)

• Record Type: Journal Article
• Authors: Sun, Jiawen; Tian, Meng; Dong, Hongchun; Lu, Zhengyi; Peng, Lin; Rong, Yi; Yang, Ruizhi; Shu, Jie; Jin, Chao
• Is Part Of: Applied materials today. Volume 27(2022)
• Publication Date: 2022-06
• Subjects: Solid state lithium battery -- Polymer-ceramic electrolytes -- LLZTO -- PESF -- Low temperature; Materials science -- Periodicals; Materials -- Research -- Periodicals; 620.1105
• DOI: 10.1016/j.apmt.2022.101447
• Languages: English
• ISSNs: 2352-9407

Abstract

Highlights: A novel "polymer in ceramic" PESF-LLZTO CPEs is reported. An amazing conductivity at −10–80 o C and an enhanced tLi+ are obtained. A strong interaction among LLZTO, PESF and wetting agent contributes to the excellent performance. SSLBs of Li||0.2PESF-0.8LLZTO CPEs||LiFePO4 demonstrate the possibility for the practical application at a wide temperature range. Abstract: Developing solid state lithium batteries (SSLBs) is an essential step to overcome current safety and energy density issues of traditional Li-ion batteries. As the core component of SSLBs, a solid electrolyte with high ionic conductivity, great physical and chemical properties is still under exploration. Herein, a novel "polymer in ceramic" composite polymer-ceramic electrolytes (CPEs) is reported, which is composed of a polyether sulfone (PESF) polymer and cubic Li6.4 La3 Zr1.4 Ta0.6 O12 (LLZTO) ceramic with high contents (up to 80 wt. %). The as-prepared PESF-LLZTO CPEs possess good heat resistance and high mechanical strength to maintain structural integrity. The optimized 0.2PESF-0.8LLZTO CPEs exhibits an excellent ionic conductivity of 4.13×10 −4 S cm −1 with a t Li + value as high as 0.64 at 20 °C after wetted by trace wetting agent (6.0 ul cm −2 ). More impressively, the ionic conductivity is still reached 1.49×10 −4 S cm −1 at -10 °C and 9.42×10 −4 S cm −1 at 80 o C. Meanwhile, the 0.2PESF-0.8LLZTO CPEs shows a broad electrochemical window (≤4.8 V vs. Li + /Li) and an excellent compatibility with Li metal. Density functional theory calculations and 6 Li solid-state NMR characterizations suggest that strong interactions among LLZTO, PESF and wetting agents contribute to the enhanced conductivity. As a proof for practical application, the Li||0.2PESF-0.8LLZTO CPEs||LiFePO4 full cells deliver a specific discharge capacity of 133.2 mAh g −1 at 2.0 C, and successfully run over 80 cycles at 0.5 C without capacity attenuation at 20 °C. The full cell also demonstrates a possibility for the application at low temperature down to -10 o C and high temperature up to 60 o C. This work brings a new perspective for high-performance SSLBs. Graphical abstract: Image, graphical abstract