原位聚合三维陶瓷骨架增强全固态锂电池电解质

有机/无机复合电解质被认为是全固态锂电池中最具潜力的固态电解质之一, 但由于无机填料易团聚, 通过提高无机填料含量来改善复合电解质的电导率难有成效。此外, 在全固态锂电池中, 电解质和电极之间松散的固-固接触造成过大的界面阻抗, 限制了全固态锂电池的性能。本研究采用固相法合成具有Li⁺连续传输通道的自支撑三维多孔Li_6.4Al_0.1La₃Zr_1.7Ta_0.3O₁₂骨架, 并利用原位聚合的方法构筑一体化电解质/电极固-固界面。此策略指导合成的复合电解质的室温电导率可达1.9×10^-4 S·cm^-1。同时, 一体化的界面使得Li-Li对称电池的界面阻抗从1540 Ω·cm ²降低至449 Ω·cm ², 因此4.3 V(vs. Li⁺/Li)的LiCoO₂|Li全固态锂电池展现出良好的电化学性能。

In-situ Polymerization Integrating 3D Ceramic Framework in All Solid-state Lithium Battery

Organic/inorganic composites have been considered as promising electrolyte candidates in all solid-state lithium batteries. Aiming at improving the conductivity significantly by increasing the frequently-used 0D or 1D ceramic nano-fillers to high content is unsuccessful due to the particle tendency to agglomeration. What's worse, the loose contact between the solid electrolyte and solid electrodes is much of a serious barrier to the performance and thus to the application of all solid-state lithium batteries. Herein, self-supported 3D porous Li_6.4Al_0.1La₃Zr_1.7Ta_0.3O₁₂ frameworks are employed to provide percolated fast Li⁺ conductive pathway while in-situ polymerization of poly(ethylene glycol) methyl ether acrylate can integrate the loose solid-solid interface and reduce the interfacial resistance efficiently. Inspiringly, the Li⁺ conductivity of the composite exhibits 1.9×10^-4 S·cm^-1 at room temperature. The interfacial resistance in Li-Li batteries decreases significantly from 1540 to 449 Ω·cm ², rendering good capacity and cyclability of the 4.3 V (vs. Li⁺/Li) LiCoO₂|Li all solid-state lithium battery.