Key Takeaways & Executive Findings
- •• In situ etching and co-growth of ultra-thin defect-rich oxide layers on porous silicon create a catalytic interface that promotes selective FEC adsorption and decomposition to a LiF-rich SEI. • The robust SEI enables high-rate performance (692 mAh g−1 at 25 A g−1) and high Coulombic efficiency (99.7% over 1000 cycles) at varied temperatures. • The catalytic interface addresses the uncontrollable SEI formation on porous silicon, overcoming limitations of conventional carbon composites and nanostructures. • This approach offers significant advantages for fast-charging silicon-based anodes in lithium-ion batteries.
Abstract
Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density. Nevertheless, the poor rate performance and limited cycling life remain unresolved through conventional approaches that involve carbon composites or nanostructures, primarily due to the un-controllable effects arising from the substantial formation of a solid electrolyte interphase (SEI) during the cycling. Here, an ultra-thin and homogeneous Ti doping alumina oxide catalytic interface is meticulously applied on the porous Si through a synergistic etching and hydrolysis process. This defect-rich oxide interface promotes a selective adsorption of fluoroethylene carbonate, leading to a catalytic reaction that can be aptly described as “molecular concentration-in situ conversion”. The resultant inorganic-rich SEI layer is electrochemical stable and favors ion-transport, particularly at high-rate cycling and high temperature. The robustly shielded porous Si, with a large surface area, achieves a high initial Coulombic efficiency of 84.7% and delivers exceptional high-rate performance at 25 A g−1 (692 mAh g−1) and a high Coulombic efficiency of 99.7% over 1000 cycles. The robust SEI constructed through a precious catalytic layer promises significant advantages for the fast development of silicon-based anode in fast-charging batteries.
1. Introduction
Silicon anodes, with high theoretical specific capacity of 3579 mAh g−1 hold a predominate position in the commercial market for high energy density lithium-ion batteries. However, huge volume change of Si (~300%) during lithiation/delithiation, always leads to capacity degradation [1, 2], demonstrating low power density and limited cycling life, especially at high temperature. On the interface of silicon, the solid electrolyte interphase (SEI) is fragile and unstable, which could not sustain the huge volume change of the silicon, would be continuous destroyed and re-formation at the repeating cycles [3, 4].
Nano-structured Si is developed to improve the ion transportation at high current density, for example, nanoparticle, nanowire, porous structure or composites. Although structural stability is improved, severe chemical reactions at the interface cannot be fully addressed through the above strategy. The large specific surface area of nanostructures and repeating side reaction would consume the electrolyte, lead to fast capacity degradation [1, 5]. The adverse reactions would accelerate at high temperatures, might precipitate thermal runaway, posing significant safety risks [6, 7]. In essence, designing the stable SEI with specific composition and structure could be achieved through electrolyte modulation and electrode design. However, devising an efficacious interfacial protection layer between the electrode and electrolyte is a critical challenge.
Recently, the interaction between electrodes and electrolytes have gathered increasing attention [8–11]. The deployment of high-concentration or localized high-concentration electrolytes can modulate the solvation structure of lithium ions, thereby engendering a stable SEI [12, 13]. Meanwhile, the incorporation of electrolyte additives to improve the interfacial stability of the electrode, such as vinylene carbonate (VC) and fluoroethylene carbonate (FEC) have been shown [14–16]. FEC, in particular, is widely used due to its higher reduction potential compared with other electrolyte components [17–19], which is decomposed to form a stable LiF-rich SEI. LiF is considered as a key inorganic component of SEI, owing to its high chemical stability and electronic insulati
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Zhuobin Han, Phornphimon Maitarad, Nuttapon Yodsin, Baogang Zhao, Haoyu Ma, Kexin Liu, Yongfeng Hu, Siriporn Jungsuttiwong, Yumei Wang, Li Lu, Liyi Shi, Shuai Yuan, Yongyao Xia, Yingying Lv (2025). Catalysis-Induced Highly-Stable Interface on Porous Silicon for High-Rate Lithium-Ion Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01701-8
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Frequently Asked Questions
What is the main challenge in using silicon anodes for lithium-ion batteries?
Silicon anodes suffer from huge volume changes (~300%) during cycling, leading to unstable solid electrolyte interphase (SEI) formation, poor rate performance, and limited cycling life, especially at high temperatures.
How does the catalytic interface improve the performance of porous silicon anodes?
The ultra-thin Ti-doped alumina oxide catalytic interface promotes selective adsorption and decomposition of fluoroethylene carbonate (FEC), resulting in a robust LiF-rich SEI that is electrochemically stable and facilitates ion transport, enabling high-rate and long-cycle performance.
What are the key performance metrics achieved in this study?
The porous silicon anode with the catalytic interface achieves an initial Coulombic efficiency of 84.7%, a high-rate capacity of 692 mAh g−1 at 25 A g−1, and a Coulombic efficiency of 99.7% over 1000 cycles.
Why is the formation of a stable SEI critical for silicon anodes?
A stable SEI prevents continuous electrolyte decomposition and electrode degradation, which are major causes of capacity fading and safety issues, especially at high temperatures and high current densities.
What is the significance of the 'molecular concentration-in situ conversion' mechanism?
This mechanism describes how the catalytic interface concentrates FEC molecules and converts them in situ into a LiF-rich SEI, ensuring a uniform and robust protective layer that enhances the electrochemical performance of silicon anodes.
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