<br>在准固态电解质中通过 LaF3 掺杂实现高通量锂离子传导,Advanced Functional Materials

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在准固态电解质中通过 LaF3 掺杂实现高通量锂离子传导
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2024-02-19 , DOI: 10.1002/adfm.202311848
Linnan Bi _{1,

2} , Liang He ₂ , Yaochen Song _{1,

2} , Yi Wang _{2,

3} , Qingyu Xie ₂ , Peng Dong ₄ , Yingjie Zhang ₄ , Yao Yao ₄ , Jiaxuan Liao _{1,

2} , Sizhe Wang _{2,

3}

Affiliation

PVDF 基电解质在室温下固有的低离子电导率和锂枝晶渗透阻碍了其进一步应用。在此，开发了一种 LaF₃ 掺杂的聚（偏二氟乙烯-三氟氯乙烯）（P（VDF-ctfe））准固体电解质。由于锂环境的优化，镧优先与阴离子物质竞争配位以放松锂跳跃，从而产生了高通量通道。因此，锂载体在分子水平上具有高度自由和未结合，在 25 °C 时产生 0.7 mS ^cm-1 的高离子电导率（σ）和 0.79 的转移数（t_Li+）。此外，原位富含有机-无机LiF的介电层有效地提高了电极/电解质界面的稳定性和兼容性，确保了界面锂的导电性，同时促进了稳定的Li⁺电镀/剥离。因此，优化的 Li/ATCSE-3%/Li 可以在 0.1 和 0.3 mA ^cm-2 下提供良好的相容性，分别用于 2000 小时和 1200 小时的稳定 Li⁺ 电镀/剥离。高质量负载（6.4 mg cm⁻²）软包池可在 100 次循环中提供稳定的循环性能，在 0.3 °C 时容量保持率为 85.8%。预计这项工作将为用于实用准固态锂金属电池的聚合物基锂传输的创造性设计提供相当大的见解。

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Realizing High-Flux Lithium-Ion Conduction by LaF3 Doping in Quasi-Solid-State Electrolytes

The inherent low ionic conductivity of PVDF-based electrolytes at room temperature and lithium dendrite penetration hinder its further application. Herein, a LaF₃ doped Poly(vinylidene fluoride-chlorotrifluoroethylene) (P(VDF-ctfe)) quasi-solid electrolyte is developed. High-flux channels are created due to the optimization of the lithium environment that lanthanum preferentially competes coordination with anionic species for relaxing lithium hopping. Lithium carriers are therefore highly free and unbound at the molecular level, resulting in a high ionic conductivity (σ) of 0.7 mS cm⁻¹ and a transfer number (t_Li+) of 0.79 at 25 °C. Moreover, the in situ organic–inorganic LiF-rich dielectric layer effectively improves the stability and compatibility of the electrode/electrolyte interface, ensuring interfacial lithium conduction while facilitating stable Li⁺ plating/stripping. As a result, the optimized Li/ATCSE-3%/Li can deliver favorable compatibility at 0.1 and 0.3 mA cm⁻² for stable Li⁺ plating/stripping for 2000 and 1200 h, respectively. The high-mass loading (6.4 mg cm⁻²) pouch cell delivers a stable cycling performance over 100 cycles with a capacity retention of 85.8% at 0.3 °C. This work is anticipated to provide considerable insight into the creative design of lithium transport of polymer-based for practical quasi-solid-state lithium metal batteries.

更新日期：2024-02-19

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