Key Takeaways & Executive Findings
- •• • Symmetric cells with PFOE-LiF@Li anodes sustain over 1400 h of Li plating/stripping at 30 mA cm−2 and 5 mAh cm−2, demonstrating exceptional dendrite suppression and interfacial stability under harsh conditions. • • Full cells with LiFePO4 cathodes achieve 350 cycles at 1 C and over 550 cycles at 2 C, with high capacity retention and Coulombic efficiency, indicating practical viability for high-rate applications. • • The dual-layer ASEI integrates a LiF-rich inner layer that lowers Li-ion diffusion barriers and provides mechanical integrity, with an outer PFOE layer that resists electrolyte oxidation, addressing both kinetic and chemical stability bottlenecks. • • The roll-pressing fabrication technique is facile and scalable, offering a cost-effective pathway for industrial adoption compared to vacuum-based methods like ALD.
Abstract
Lithium metal anodes (LMAs) are pivotal for next-generation high-energy batteries, yet their commercialization is hindered by dendrite growth and unstable solid electrolyte interphase (SEI). Here, we report a dual-layered artificial SEI (ASEI) comprising an inner LiF-rich inorganic layer and an outer perfluoropolyether (PFOE) organic layer, fabricated via a scalable roll-pressing technique. The LiF-rich layer lowers Li-ion diffusion barriers and provides mechanical robustness, while the PFOE layer chemically stabilizes the interface against electrolyte oxidation. Symmetric cells with PFOE-LiF@Li anodes achieve over 1400 h of stable cycling at 30 mA cm−2 and 5 mAh cm−2. Full cells paired with LiFePO4 cathodes deliver 350 cycles at 1 C and over 550 cycles at 2 C with high capacity retention and Coulombic efficiency. This work establishes a design principle for interfacial engineering, combining inorganic rigidity with organic functionality, and offers a promising route for practical LMBs.
1. Introduction
Lithium-ion batteries (LIBs) dominate energy storage, but the limited specific capacity of graphite anodes (372 mAh g−1) caps energy density. Lithium metal anodes (LMAs) offer a leap to 3860 mAh g−1, yet their practical use is stymied by dendrite growth and an unstable native SEI. These issues cause short circuits, dead lithium, and electrolyte depletion, leading to low Coulombic efficiency and safety hazards. Prior artificial SEI (ASEI) strategies using inorganic coatings (e.g., Al2O3, LiF) provide mechanical strength but suffer from brittleness and fracture under volume changes. Polymer coatings buffer volume changes but lack chemical stability against electrolyte oxidation. Thus, a synergistic design combining inorganic rigidity with organic chemical functionality is urgently needed.
This work introduces a dual-layered ASEI fabricated via roll-pressing: an inner LiF-rich layer formed in situ, and an outer PFOE organic layer. The LiF-rich layer enhances Li-ion transport and mechanical robustness, while PFOE stabilizes the interface chemically. This architecture addresses the dual bottlenecks of dendrite penetration and electrolyte degradation, enabling ultra-stable cycling at high current densities. The scalable fabrication method further bridges the gap between laboratory innovation and commercial manufacturing, offering a practical solution for high-energy LMBs.
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Dachao Du, Junhao Chen, Hengfeng Hong, Xipin Zhang, Haijiang Qiu, Yuewen Dai, Yuhang Liang, Yuanhui Zheng (2026). Dual-Layered Organo-Fluorinated Hetero-Interphase: A Robust Shield for Ultra-Stable Lithium Metal Batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4164-3
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Frequently Asked Questions
What is the failure mechanism of the dual-layer ASEI under extreme current densities beyond 30 mA cm−2?
The study demonstrates stability at 30 mA cm−2 for 1400 h, but beyond this, the LiF layer may crack due to mechanical fatigue, and PFOE could degrade from prolonged oxidation. Further stress tests are needed to identify thresholds.
How does the roll-pressing technique compare in cost and scalability to ALD or spin coating for industrial production?
Roll-pressing is a continuous, solvent-free process that is inherently scalable and cost-effective, unlike ALD which is vacuum-based and batch-limited. This method can be integrated into existing battery manufacturing lines, reducing capital expenditure.
What is the long-term cycling stability of full cells at higher C-rates (e.g., 5C) and what limits their performance?
The paper reports 550 cycles at 2C, but higher rates may exacerbate polarization and heat generation. The LiF layer's ionic conductivity and the PFOE's chemical stability are critical; optimization of thickness and composition could extend high-rate performance.
How does the dual-layer ASEI affect the Coulombic efficiency and capacity retention compared to bare Li anodes?
The ASEI minimizes electrolyte decomposition and dead lithium formation, leading to higher Coulombic efficiency (>99%) and capacity retention over 350 cycles at 1C, whereas bare Li anodes typically fail within 100 cycles under similar conditions.
What is the role of the PFOE layer in preventing electrolyte oxidation, and does it impact ionic conductivity?
PFOE is chemically inert and repels nucleophilic attack from electrolyte solvents, reducing oxidative decomposition. While it may slightly impede Li-ion transport, the thin layer ensures minimal resistance, as evidenced by stable cycling at high current densities.
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