Issue

Vol. 19 (2027)

High-Conductivity and Moisture-Tolerant Sulfide Electrolyte Enabled by Bifunctional Coating for Practical All-Solid-State Lithium Batteries

https://doi.org/10.1007/s40820-026-02353-y
Dabing Li
School of Materials Science and Engineering, State Center for International Cooperation on Designer Low‑carbon and Environmental Materials (CDLCEM), Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Hongjie Xu
School of Materials Science and Engineering, North China University of Water Resources and Electric Power, Zhengzhou 450046, People’s Republic of China
Guoqin Cao
School of Materials Science and Engineering, State Center for International Cooperation on Designer Low‑carbon and Environmental Materials (CDLCEM), Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Fanfan Liu
School of Materials Science and Engineering, State Center for International Cooperation on Designer Low‑carbon and Environmental Materials (CDLCEM), Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Jinjin Ban
School of Materials Science and Engineering, State Center for International Cooperation on Designer Low‑carbon and Environmental Materials (CDLCEM), Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Shilin Zhang
School of Materials Science and Engineering, State Center for International Cooperation on Designer Low‑carbon and Environmental Materials (CDLCEM), Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Li‑Zhen Fan
Institute of Advanced Materials and Technology, University of Science and Technology Beijing, Beijing 100083, People’s Republic of China
Junhua Hu
School of Materials Science and Engineering, State Center for International Cooperation on Designer Low‑carbon and Environmental Materials (CDLCEM), Zhengzhou University, Zhengzhou 450001, People’s Republic of China

Corresponding Author: Junhua Hu

hujh@zzu.edu.cn

Nano-Micro Letters, Vol. 19 (2027), Article Number: 51

Abstract

The pursuit of safer and higher-energy-density batteries has driven the advancement of all-solid-state lithium batteries (ASSLBs). Among various material systems, sulfide solid-state electrolytes (SEs) stand out as highly promising candidates owing to their exceptional ionic conductivity. Nevertheless, their extreme sensitivity to moisture results in the release of toxic H2S and rapid structural degradation, which severely impedes their scalable manufacturing under ambient conditions. A bifunctional (3-mercaptopropyl)trimethoxysilane (MPTMS) coating strategy is herein presented to shield Li5.5PS4.5Cl0.8Br0.7 (LPSCBr) from moisture-induced degradation. The MPTMS layer forms a hydrophobic barrier of approximately 10 nm, which reduces H2S emission by 93.0% after 35 min of exposure to 30% relative humidity, while maintaining 83.1% of the initial ionic conductivity (10.8 mS cm−1). This approach tackles the core challenge associated with sulfide solid-state electrolytes: the realization of compatibility with controlled ambient air without sacrificing critical electrochemical properties. The modified electrolyte maintains a high ionic conductivity (> 5.7 mS cm−1) even after 10 h of air exposure. When applied in all-solid-state cells paired with LiNi0.83Co0.11Mn0.06O2 cathodes, it exhibits remarkable electrochemical performance, delivering a capacity retention of 84.6% after 1000 cycles. By enabling moisture-tolerant processing, MPTMS-modified LPSCBr SEs lay a solid foundation for the scalable, high-performance, and cost-effective production of ASSLBs.


Highlights:
1 (3-Mercaptopropyl)trimethoxysilane (MPTMS) forms a hydrophobic coating on Li5.5PS4.5Cl0.8Br0.7 (LPSCBr) via synergistic covalent bonding of dual functional groups (–SH and –Si(OCH3)3).
2 The siloxane network blocks moisture, and S–S bonds stabilize the PS43− framework to inhibit electrolyte hydrolysis fundamentally.
3 The bifunctional MPTMS coating on LPSCBr simultaneously enhances electrolyte moisture resistance and cathode interfacial stability.

Keywords

All-solid-state lithium batteries Sulfide electrolytes Surface modification Moisture tolerance Long cycling stability
Li, Dabing, Hongjie Xu, Guoqin Cao, Fanfan Liu, Jinjin Ban, Shilin Zhang, Li‑Zhen Fan, and Junhua Hu. 2026. “High-Conductivity and Moisture-Tolerant Sulfide Electrolyte Enabled by Bifunctional Coating for Practical All-Solid-State Lithium Batteries”. Nano-Micro Letters 19 (October):51. https://doi.org/10.1007/s40820-026-02353-y.
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