3D-Printed PMMA-Regulated PAN-Based Gel Polymer Electrolytes for Lithium Metal Batteries

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Abstract
Gel polymer electrolytes (GPEs) have emerged as promising electrolytes for lithium metal batteries owing to their high ionic conductivity, mechanical flexibility, and reduced risk of electrolyte leakage. However, PAN-based GPEs still suffer from limited ion transport caused by the semi-crystalline structure of PAN chains. In this work, polyacrylonitrile (PAN)/poly(methyl methacrylate) (PMMA)/lithium aluminum titanium phosphate (LATP)/lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) gel polymer electrolytes were fabricated via direct ink writing (DIW) 3D printing, where PMMA was introduced to regulate the PAN matrix and enhance Li+ transport. The results reveal that PMMA incorporation effectively reduces PAN crystallinity, increases the amorphous fraction, and modifies the local functional-group environment of the polymer matrix, while LATP fillers further improve ionic transport and mechanical stability. The optimized PPM8:2 gel polymer electrolyte delivers a room-temperature ionic conductivity of 4.22 × 10−4 S cm−1, a Li+ transference number of 0.624, and an electrochemical stability window of 4.75 V. When applied in LiFePO4|Li batteries, it maintains a discharge capacity of approximately 150 mAh g−1 after 100 cycles at 0.1 C with excellent rate capability and cycling stability. This work provides an effective approach to developing PAN-based gel polymer electrolytes for high-performance lithium metal batteries.
Funding Information
  • National Natural Science Foundation of China (22462003)
  • Guangxi Key R&D Program Projects (AB24010346)
  • Guangxi Key Laboratory of Automobile Components and Vehicle Technology (2023GKLACVTZZ02)
  • Guangxi Key Laboratory of Automobile Components and Vehicle Technology (2022GKLACVTZZ04)
  • Guangxi Key Laboratory of Automobile Components and Vehicle Technology (2023GKLACVTZZ10)
  • Innovation Project of Guangxi Graduate Education (YCSW2025576)
  • Guangxi University of Science and Technology (23Z04)
  • Innovation Project of Guangxi University of Science and Technology Graduate Education (GKYC202565)

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