Key Takeaways & Executive Findings
- •• Uniform and stable interfacial layer with both ionic and electronic conduction on the surface of solid-state composite cathode by in situ polymerization cyclization treatment. • Theoretical calculations demonstrate that cPAN can effectively inhibit transition metal dissolution and uneven cyclic stress distribution and improve the stability of the crystal structure. • In-cPAN-260@NCM811 has excellent cycling performance with 86.8% retention after 300 cycles and thermally safe stability at high-temperature extremes. • The facile and scalable surface engineering approach represents significant progress in developing high-performance solid-state lithium metal batteries.
Abstract
High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density, but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes. To circumvent these issues, a continuous uniform layer polyacrylonitrile (PAN) was introduced on the surface of LiNi0.8Mn0.1Co0.1O2 via in situ polymerization of acrylonitrile (AN). Furthermore, the partial-cyclized treatment of PAN (cPAN) coating layer presents high ionic and electron conductivity, which can accelerate interfacial Li+ and electron diffusion simultaneously. And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation, which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode. Besides, the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure. Benefited from these, the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8% after 300 cycles and superior rate capability. And endow the solid-state battery with thermal safety stability even at high-temperature extreme environment. This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.
1. Introduction
Lithium-ion batteries (LIBs) face the development requirements of high-energy density and high safety. Besides, LIBs are required to operate under extreme temperature in specialized fields such as underground exploration, aerospace, and weaponry. However, high-temperature working environments can exacerbate the risk of thermal runaway in batteries due to the flammability of traditional liquid electrolytes and exothermic decomposition of active materials [1–3]. Solid-state lithium batteries (SSLBs) considered to be the most prospective next-generation battery technology with high theoretical energy density and high safety even at high temperature [4–7]. And solid-state electrolytes (SEs) act as a critical component in SSLBs, which becomes a research hotspot [8, 9]. Among various SEs, poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) based electrolytes have been widely researched and demonstrated to be promising electrolyte system due to their high ionic conductivity and good electrochemical stability [10, 11]. However, the severe cathode interface issues between high-voltage cathode and PVDF-HFP based electrolytes still hinder the further development of the SSLBs. And high-temperature working environments can accelerate the deterioration of the cathode interface, resulting in the failure of SSLBs. Thus, the promise of SSLBs has stimulated extensive research for constructing excellent cathode interface with high-voltage cathode to meet the increasing demands of high-energy–density and high safety SSLBs [12].
Among various high-voltage cathode materials, the layered oxide cathodes, especially the Ni-rich NCM cathodes (e.g., LiNi0.8Mn0.1Co0.1O2, NCM811) are considered as the ideal material in SSLBs due to their low cost and high specific capacity [13, 14]. However, the high-nickel content and the further increase of charging voltage have caused many problems, such as poor thermal stability, structural degradation, and the de...
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Jiayi Zheng, Haolong Jiang, Xieyu Xu, Jie Zhao, Xia Ma, Weiwei Sun, Shuangke Liu, Wei Xie, Yufang Chen, ShiZhao Xiong, Hui Wang, Kai Xie, Yu Han, Maoyi Yi, Chunman Zheng, Qingpeng Guo (2025). In Situ Partial-Cyclized Polymerized Acrylonitrile-Coated NCM811 Cathode for High-Temperature ≥ 100 °C Stable Solid-State Lithium Metal Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01683-7
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Frequently Asked Questions
What is the main challenge addressed in this paper?
The main challenge is the structural instability and detrimental side reactions of high-nickel ternary cathodes (NCM811) in solid-state lithium metal batteries, especially at high temperatures, which limit their performance and safety.
How does the cPAN coating improve the cathode performance?
The cPAN coating provides high ionic and electronic conductivity, accelerates interfacial Li+ and electron diffusion, inhibits side reactions with solid-state electrolytes, and provides homogeneous stress to prevent bulk structural degradation, thereby enhancing mechanical and electrochemical stability.
What is the cycling performance of the modified cathode?
The In-cPAN-260@NCM811 cathode exhibits excellent cycling performance with 86.8% capacity retention after 300 cycles, along with superior rate capability and thermal safety stability even at high-temperature extremes.
What is the significance of this work for solid-state batteries?
This work presents a facile and scalable surface engineering strategy that significantly improves the performance and safety of solid-state lithium metal batteries, representing a major step toward their practical application in high-energy-density and high-safety energy storage systems.
What are the key materials used in this study?
The key materials include LiNi0.8Mn0.1Co0.1O2 (NCM811) as the cathode, polyacrylonitrile (PAN) as the coating material, and PVDF-HFP-based solid-state electrolytes.
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