Zhao Yifan, Zhang Liang, Liu Qian, Liu Mingyu, Shen Jiajia, Ma Hui, Dai Juejing, Yu Xi, Yan Jianhua
College of Textiles, Donghua University, Shanghai, 201620, China.
School of Textile Materials and Engineering, Wuyi University, Jiangmen, 529020, China.
Adv Sci (Weinh). 2025 Aug;12(32):e06636. doi: 10.1002/advs.202506636. Epub 2025 Jun 4.
Prelithiation emerges as an effective technique to enhance the initial Coulombic efficiency (ICE) and cycling stability of silicon oxide based carbon composite (C/SiO) anodes, yet traditional approaches remain plagued by sluggish kinetics, cumbersome procedures, safety hazards, and inadequate precision. Here, a facile topological intercalation prelithiation method capable of forming a robust and homogeneous solid electrolyte interface (SEI) network on porous C/SiO nanofiber anodes in merely 30 s is reported. Through constructing three charge-driven topology models derived from flexible SiO/porous carbon nanofiber (SiO/PCNF) films, the mechanism of this fast Li-intercalation process is unraveled. Abundant surface defects on SiO/PCNF enhance lithium salt adsorption and dissociation, while the active solvated Li-ions can quickly intercalate into SiO/PCNF along an orientation pathway, realizing a high ICE of 99.44%. This topological prelithiation forges a 3D inorganic-rich SEI architecture that dualizes functionality: It curtails electrolyte degradation while alleviating volume fluctuation and mechanical stress, while enabling precision Li-ion replenishment. This topochemical paradigm not only achieves ICE reinforcement and cycling resilience (1000 stable cycles), but also slashes prelithiation duration by orders of magnitude.
预锂化成为一种提高基于氧化硅的碳复合材料(C/SiO)阳极初始库仑效率(ICE)和循环稳定性的有效技术,但传统方法仍存在动力学缓慢、程序繁琐、安全隐患和精度不足等问题。在此,报道了一种简便的拓扑插层预锂化方法,该方法能够在仅30秒内在多孔C/SiO纳米纤维阳极上形成坚固且均匀的固体电解质界面(SEI)网络。通过构建从柔性SiO/多孔碳纳米纤维(SiO/PCNF)薄膜衍生的三种电荷驱动拓扑模型,揭示了这种快速锂嵌入过程的机制。SiO/PCNF上丰富的表面缺陷增强了锂盐的吸附和解离,而活性溶剂化锂离子可以沿着取向路径快速嵌入SiO/PCNF,实现了99.44%的高ICE。这种拓扑预锂化形成了一种三维富无机SEI结构,具有双重功能:它减少了电解质降解,同时减轻了体积波动和机械应力,同时实现了精确的锂离子补充。这种拓扑化学范式不仅实现了ICE增强和循环弹性(1000次稳定循环),而且将预锂化持续时间缩短了几个数量级。