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Vol. 18 (2026)

Lithium-Ion Dynamic Interface Engineering of Nano-Charged Composite Polymer Electrolytes for Solid-State Lithium-Metal Batteries

https://doi.org/10.1007/s40820-025-01899-7
Shanshan Lv
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
Jingwen Wang
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
Yuanming Zhai
Analytical and Testing Center, Sichuan University, Chengdu 610065, People’s Republic of China
Yu Chen
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
Jiarui Yang
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
Zhiwei Zhu
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
Rui Peng
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
Xuewei Fu
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
http://orcid.org/0000-0002-1164-427X
Wei Yang
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China
Yu Wang
College of Polymer Science and Engineering, National Key Laboratory of Advanced Polymer Materials, Sichuan University, Chengdu 610065, People’s Republic of China

Corresponding Author: Yu Wang

yu.wang3@scu.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 46

Abstract

Composite polymer electrolytes (CPEs) offer a promising solution for all-solid-state lithium-metal batteries (ASSLMBs). However, conventional nanofillers with Lewis-acid–base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously. Here, by regulating the surface charge characteristics of halloysite nanotube (HNT), we propose a concept of lithium-ion dynamic interface (Li+-DI) engineering in nano-charged CPE (NCCPE). Results show that the surface charge characteristics of HNTs fundamentally change the Li+-DI, and thereof the mechanical and ion-conduction behaviors of the NCCPEs. Particularly, the HNTs with positively charged surface (HNTs+) lead to a higher Li+ transference number (0.86) than that of HNTs− (0.73), but a lower toughness (102.13 MJ m−3 for HNTs+ and 159.69 MJ m−3 for HNTs−). Meanwhile, a strong interface compatibilization effect by Li+ is observed for especially the HNTs+-involved Li+-DI, which improves the toughness by 2000% compared with the control. Moreover, HNTs+ are more effective to weaken the Li+-solvation strength and facilitate the formation of LiF-rich solid–electrolyte interphase of Li metal compared to HNTs−. The resultant Li|NCCPE|LiFePO4 cell delivers a capacity of 144.9 mAh g−1 after 400 cycles at 0.5 C and a capacity retention of 78.6%. This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.


Highlights:
1 The surface charge characteristics of halloysite nanotubes (HNTs) are manipulated to engineer the Li+-dynamic interface (Li+-DI) in composite polymer electrolytes.
2 Surface charge characteristics of HNTs generate pronounced impact on not only the ionic/mechanical properties of the composite electrolytes, but also the formation and composition of solid–electrolyte interphase (SEI) layer.
3 HNTs+-supported Li+-DI exhibits an anion-rich Li+-solvation structure and soft-and-tough mechanical interface, leading to LiF-rich SEI layer and improvement of toughness by over 2000% compared with the control.

Keywords

Charged nanofillers Nanocomposite polymer electrolyte Dynamic lithium ion interface Solid ion-conductors Solid-state lithium-metal battery
Lv, Shanshan, Jingwen Wang, Yuanming Zhai, Yu Chen, Jiarui Yang, Zhiwei Zhu, Rui Peng, Xuewei Fu, Wei Yang, and Yu Wang. 2025. “Lithium-Ion Dynamic Interface Engineering of Nano-Charged Composite Polymer Electrolytes for Solid-State Lithium-Metal Batteries”. Nano-Micro Letters 18 (August):46. https://doi.org/10.1007/s40820-025-01899-7.
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