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High‐Performance Silicon Anodes Enabled by Multifunctional Ultrafine Silica Nanoparticle‐Embedded Carbon Coatings for Lithium‐Ion Batteries

Zhefei SunState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaQuanzhi YinState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaShenghui ZhouState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaHaoyu ChenState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaSifan WenState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaHuiping YangState Key Laboratory of Material Processing and Die & Mould Technology Department of Mechanics School of Aerospace Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 ChinaXiaoyu WuState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaJianhai PanState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaJiajia HanState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaHui Ying YangState Key Laboratory of Material Processing and Die & Mould Technology Department of Mechanics School of Aerospace Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 ChinaZilong ZhuangDepartment of Mechanical Engineering University of Wisconsin‐Madison Madison WI 53706 USAShijie FengMaterials Science and Engineering Program University of California San Diego La Jolla CA 92093 USALi ZhangState Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Tan Kah Kee Innovation Laboratory Collaborative Innovation Center of Chemistry for Energy Materials Xiamen University Xiamen Fujian 361005 ChinaDong‐Liang PengState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361005 ChinaQiaobao ZhangLongmen Laboratory Luoyang Henan 471023 China
2025en
ABI

Аннотация

Abstract Silicon (Si) holds immense promise as viable anode for next‐generation high‐energy‐density Li‐ion batteries (LIBs). However, its poor ionic/electronic conductivity and significant volumetric changes during cycling lead to rapidly deteriorated LIB performance. Here, a novel multifunctional coating featuring ultrafine SiO 2 nanoparticles (<7 nm) embedded carbon on Si nanoparticles (termed Si@uSiO 2 ‐C) to resolve these challenges is proposed. This unique uSiO 2 ‐C coating provides high‐efficient electron and ion transport pathways, while also improves interfacial stability and mitigates volume changes during cycling, thereby enhancing the conductivity and structural integrity of Si@uSiO 2 ‐C, as corroborated by extensive experimental and computational studies. In addition, the abundant interfaces in uSiO 2 ‐C coating facilitate Li + transport and the evenly distributed ultrafine SiO 2 nanoparticles impart high electrochemical reactivity and mechanical robustness. Consequently, the Si@uSiO 2 ‐C anode achieves a high reversible capacity of 2093 mAh g −1 at 0.2 A g −1 , with a high initial Coulombic efficiency of 88.3%, superior rate capability and durability (1000 cycles, 928 mAh g −1 at 1.0 A g −1 , 75% capacity retention). Full cells paired with commercial LiFePO 4 cathodes demonstrate high cyclability, maintaining 80% capacity retention over 500 cycles at 4 C. This work highlights the vital role of multifunctional coating in promoting the electrochemical performance of Si‐based anodes for high‐performance LIBs.

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