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Vol. 17 (2025)

A Mechanically Robust In-Situ Solidified Polymer Electrolyte for SiOx-Based Anodes Toward High-Energy Lithium Batteries

https://doi.org/10.1007/s40820-025-01759-4
Cizhen Luo
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, People’s Republic of China
Huanrui Zhang
Qingdao Institute of Bioenergy and Bioprocess Technology, Qingdao Industrial Energy Storage Research Institute, Chinese Academy of Science, Qingdao 266101, People’s Republic of China
Chenghao Sun
Qingdao Institute of Bioenergy and Bioprocess Technology, Qingdao Industrial Energy Storage Research Institute, Chinese Academy of Science, Qingdao 266101, People’s Republic of China
Xing Chen
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, People’s Republic of China
Wenjun Zhang
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, People’s Republic of China
Pengzhou Mu
Qingdao Institute of Bioenergy and Bioprocess Technology, Qingdao Industrial Energy Storage Research Institute, Chinese Academy of Science, Qingdao 266101, People’s Republic of China
Gaojie Xu
Qingdao Institute of Bioenergy and Bioprocess Technology, Qingdao Industrial Energy Storage Research Institute, Chinese Academy of Science, Qingdao 266101, People’s Republic of China
Rongxian Wu
Qingdao Institute of Bioenergy and Bioprocess Technology, Qingdao Industrial Energy Storage Research Institute, Chinese Academy of Science, Qingdao 266101, People’s Republic of China
Zhaolin Lv
Qingdao Institute of Bioenergy and Bioprocess Technology, Qingdao Industrial Energy Storage Research Institute, Chinese Academy of Science, Qingdao 266101, People’s Republic of China
Xinhong Zhou
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, People’s Republic of China
Guanglei Cui
Qingdao Institute of Bioenergy and Bioprocess Technology, Qingdao Industrial Energy Storage Research Institute, Chinese Academy of Science, Qingdao 266101, People’s Republic of China

Corresponding Author: Guanglei Cui

cuigl@qibebt.ac.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 250

Abstract

Silicon suboxide (SiOx, 0 < x < 2) is an appealing anode material to replace traditional graphite owing to its much higher theoretical specific capacity enabling higher-energy-density lithium batteries. Nevertheless, the huge volume change and rapid capacity decay of SiOx electrodes during cycling pose huge challenges to their large-scale practical applications. To eliminate this bottleneck, a dragonfly wing microstructure-inspired polymer electrolyte (denoted as PPM-PE) is developed based on in-situ polymerization of bicyclic phosphate ester- and urethane motif-containing monomer and methyl methacrylate in traditional liquid electrolyte. PPM-PE delivers excellent mechanical properties, highly correlated with the formation of a micro-phase separation structure similar with dragonfly wings. By virtue of superior mechanical properties and the in-situ solidified preparation method, PPM-PE can form a 3D polymer network buffer against stress within the electrode particles gap, enabling much suppressed electrode volume expansion and more stabilized solid electrolyte interface along with evidently decreased electrolyte decomposition. Resultantly, PPM-PE shows significant improvements in both cycling and rate performance in button and soft package batteries with SiOx-based electrodes, compared with the liquid electrolyte counterpart. Such a dragonfly wing microstructure-inspired design philosophy of in-situ solidified polymer electrolytes helps facilitate the practical implementation of high-energy lithium batteries with SiOx-based anodes.


Highlights:
1 Inspired by the microstructure of high-mechanical-property dragonfly wings, a phase separation structure design philosophy of in-situ solidified polymer electrolytes was first proposed, enabling superior mechanical properties of them.
2 By virtue of superior mechanical properties and the in-situ solidified preparation method, the failure behaviors of SiOx-based electrodes are effectively suppressed by the as-developed polymer electrolyte.
3 A dragonfly wing microstructure-inspired polymer electrolyte (denoted as PPM-PE) enables excellent electrochemical performance of SiOx-based electrodes in button-type and soft package full cells.

Keywords

High-energy lithium batteries SiOx-based anodes Polymer electrolyte Micro-phase separation structure Cycle performance
Luo, Cizhen, Huanrui Zhang, Chenghao Sun, Xing Chen, Wenjun Zhang, Pengzhou Mu, Gaojie Xu, Rongxian Wu, Zhaolin Lv, Xinhong Zhou, and Guanglei Cui. 2025. “A Mechanically Robust In-Situ Solidified Polymer Electrolyte for SiOx-Based Anodes Toward High-Energy Lithium Batteries”. Nano-Micro Letters 17 (May):250. https://doi.org/10.1007/s40820-025-01759-4.
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