An Advanced Gel Polymer Electrolyte for Solid-State Lithium Metal Batteries

Chunxiang Xian; Shengzhao Zhang; Ping Liu; Lei Huang; Xinping He; Shenghui Shen; Feng Cao; Xinqi Liang; Chen Wang; Wangjun Wan; Yongqi Zhang; Xin Liu; Yu Zhong; Yang Xia; Minghua Chen; Wenkui Zhang; Xinhui Xia; Jiangping Tu

doi:10.1002/smll.202306381

An Advanced Gel Polymer Electrolyte for Solid-State Lithium Metal Batteries

Small. 2024 Apr;20(15):e2306381. doi: 10.1002/smll.202306381. Epub 2023 Nov 27.

Authors

Chunxiang Xian¹, Shengzhao Zhang¹, Ping Liu¹, Lei Huang¹, Xinping He², Shenghui Shen³, Feng Cao⁴, Xinqi Liang^{1

5

6}, Chen Wang⁷, Wangjun Wan⁷, Yongqi Zhang⁵, Xin Liu⁸, Yu Zhong¹, Yang Xia², Minghua Chen⁶, Wenkui Zhang², Xinhui Xia^{1

2

9}, Jiangping Tu¹

Affiliations

¹ School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, P. R. China.
² College of Materials Science & Engineering, Zhejiang University of Technology, Hangzhou, 310014, China.
³ School of Materials Science and & Engineering, Zhejiang Sci-Tech University, Hangzhou, 310018, China.
⁴ Department of Engineering Technology, Huzhou College, Huzhou, 313000, P. R. China.
⁵ Institute of Fundamental and Frontier Science, University of Electronic Science and Technology of China, Chengdu, 611371, China.
⁶ Key Laboratory of Engineering Dielectric and Applications (Ministry of Education), School of Electrical and Electronic Engineering, Harbin University of Science and Technology, Harbin, 150080, P. R. China.
⁷ Zhejiang Academy of Science and Technology for Inspection & Quarantine, Zhejiang, Hangzhou, 311215, P. R. China.
⁸ State Key Laboratory of New Textile Materials and Advanced Processing Technologies, Wuhan Textile University, Wuhan, 430200, China.
⁹ State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou, 350116, China.

PMID: 38013253
DOI: 10.1002/smll.202306381

Abstract

All-solid-state lithium metal batteries (LMBs) are regarded as one of the most viable energy storage devices and their comprehensive properties are mainly controlled by solid electrolytes and interface compatibility. This work proposes an advanced poly(vinylidene fluoride-hexafluoropropylene) based gel polymer electrolyte (AP-GPEs) via functional superposition strategy, which involves incorporating butyl acrylate and polyethylene glycol diacrylate as elastic optimization framework, triethyl phosphate and fluoroethylene carbonate as flameproof liquid plasticizers, and Li₇La₃Zr₂O₁₂ nanowires (LLZO-w) as ion-conductive fillers, endowing the designed AP-GPEs/LLZO-w membrane with high mechanical strength, excellent flexibility, low flammability, low activation energy (0.137 eV), and improved ionic conductivity (0.42 × 10^-3 S cm^-1 at 20 °C) due to continuous ionic transport pathways. Additionally, the AP-GPEs/LLZO-w membrane shows good safety and chemical/electrochemical compatibility with the lithium anode, owing to the synergistic effect of LLZO-w filler, flexible frameworks, and flame retardants. Consequently, the LiFePO₄/Li batteries assembled with AP-GPEs/LLZO-w electrolyte exhibit enhanced cycling performance (87.3% capacity retention after 600 cycles at 1 C) and notable high-rate capacity (93.3 mAh g^-1 at 5 C). This work proposes a novel functional superposition strategy for the synthesis of high-performance comprehensive GPEs for LMBs.

Keywords: Li7La3Zr2O12 nanowire; functional superposition strategy; gel polymer electrolyte; solid‐state batteries.

Abstract

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