Zhang Tao, Li Jiafeng, Li Xiaoxuan, Wang Rutao, Wang Chengxiang, Zhang Zhiwei, Yin Longwei
Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Ji'nan, 250061, P. R. China.
Adv Mater. 2022 Oct;34(41):e2205575. doi: 10.1002/adma.202205575. Epub 2022 Sep 7.
Developing quasi-solid-state electrolytes with superior ionic conductivity and high mechanical strength is urgently desired to improve the safety and cycling stability of lithium-metal batteries. Herein, a novel solid-like electrolyte (SLE) with enhanced Li interfacial transfer kinetics is rationally designed by soaking bulk nanostructured silica-polymer composites in liquid electrolytes. Benefiting from the high content of inorganic silica and abundant interfaces for fast Li -transport channels, the prepared SLE exhibits superb ionic conductivity and high mechanical strength. Furthermore, fumed silica with a high specific area in the SLE can homogenize Li flux and electrical field gradient. More importantly, a Li S-rich solid electrolyte interphase (SEI) is constructed on the lithium metal due to the intimate ion coordination in the SLE. Therefore, the lithium-metal anode exhibits excellent electrochemical performance in symmetric Li-Li cells due to the merits of superior ionic conductivity, high modulus, Li S-rich SEI, as well as the homogeneous Li flux. Full cells with LiFePO cathode can still display a capacity retention of 98% at 0.2 C after 400 cycles. The proposed strategy on quasi-solid-state electrolytes provides a promising avenue for next-generation metal-based batteries.
迫切需要开发具有优异离子导电性和高机械强度的准固态电解质,以提高锂金属电池的安全性和循环稳定性。在此,通过将块状纳米结构二氧化硅-聚合物复合材料浸泡在液体电解质中,合理设计了一种具有增强锂界面转移动力学的新型类固体电解质(SLE)。得益于高含量的无机二氧化硅和丰富的界面提供快速锂传输通道,所制备的SLE表现出卓越的离子导电性和高机械强度。此外,SLE中具有高比表面积的气相二氧化硅可以使锂通量和电场梯度均匀化。更重要的是,由于SLE中紧密的离子配位作用,在锂金属上构建了富含硫化锂的固体电解质界面(SEI)。因此,锂金属负极在对称锂-锂电池中表现出优异的电化学性能,这得益于其卓越的离子导电性、高模量、富含硫化锂的SEI以及均匀的锂通量。具有磷酸铁锂正极的全电池在0.2 C下循环400次后仍能保持98%的容量保持率。所提出的准固态电解质策略为下一代金属基电池提供了一条有前景的途径。