有机-无机电解质复合被认为是提高固态电解质整体性能的有效措施。然而, 简单地将粉末材料填料添加到有机聚合物中并不能显著提高电解质的机械性能。
近日,华中科技大学李会巧教授、王书豪博士、江汉大学刘喜正教授和浙江锋锂新能源科技有限公司崔言明博士等人在Science China Materials发表研究论文,设计了一种超薄、高机械强度和离子电导率的有机-无机复合固态电解质,其中无机固态电解质(Li1.5Al0.5Ge1.5(PO4)3, LAGP)被预纤维化成一个三维纳米网络骨架,预纤维化的LAGP作为聚氧化乙烯(PEO)基质的自支撑骨架。
本文要点
1) 连续的骨架结构不仅显著提高了PEO基电解质的机械强度,还形成了一个连续的锂离子传导路径,促进了锂离子的快速迁移。2) 纤维增强的复合电解质膜在60°C时的离子电导率为8.27×10−4 S cm−1,拉伸强度高达4.29 MPa。3) 当用于Li/Li对称电池时,它表现出较低的过电势和超过1700 h的循环稳定性。组装的LiFePO4(LFP)|Li电池在0.5 C电流下经过300个循环后比容量为142 mAh g−1,循环稳定性良好。该工作为设计下一代安全可靠的有机-无机复合固态电解质膜提供了新思路。Figure 1. Structure design and morphology of CSEs. (a) Schematic structure of the PEO-LAGP Particle electrolyte and the PEO-LAGP Fiber electrolyte. (b) Schematic diagram of the preparation of PEO-LAGP Fiber electrolyte. (c) SEM images of the LAGP nanofibers. (d) SEM images and EDS mapping of a single LAGP nanofiber. SEM images and optical photographs of (e) the PEO-LAGP Fiber electrolyte and (f) the PEO-LAGP Particle electrolyte.Figure 2. Ionic conductivity analysis of CSEs with different structure. (a) Arrhenius plots, (b) DSC curves and (c) The illustration for Li+ conduction pathways of the PEO electrolyte, the PEO-LAGP Particle electrolyte and the PEO-LAGP Fiber electrolyte.Figure 3. Lithium/lithium symmetrical cell performance of CSEs with different structure. (a) Voltage profiles of Li/PEO/Li, Li/PEO-LAGP Particle/Li and Li/PEO-LAGP Fiber/Li cells in Li plating/stripping cycles at a current density of 0.1 mA cm−2, with magnified graphs showing details from 300–304 h and 1000–1004 h. (b) Comparison of overpotentials and (c) EIS spectra of Li/PEO/Li, Li/PEO-LAGP Particle/Li and Li/PEO-LAGP Fiber/Li cells after cycling 300 cycles. (d) Voltage profile of the Li/PEO-LAGP Fiber electrolyte/Li cell in Li plating/stripping cycles at a capacity of 0.1 mAh cm−2. The cycle was carried out at 60°C.Figure 4. Li/LFP full cell performance of CSEs with different structure. (a–c) Charge/discharge curves at different cycles, (d) cycling performances and (d) rate performances of Li/LFP cells with the PEO electrolyte, the PEO-LAGP Particle electrolyte and the PEO-LAGP Fiber electrolyte at 0.2 C. (f) Cycling performance of Li/LFP cell with the PEO-LAGP Fiber electrolyte at 0.5 C. The cycle was carried out at 60°C.Shiya Li, Shuhao Wang, Gaofeng Du, Jianing Liang, Zhaoming Tong, Yanming Cui, Jiu Lin, Xiaoxiong Xu, Xizheng Liu, Tianyou Zhai, Huiqiao Li. Ultrathin inorganic-organic solid-state electrolyte reinforced by a pre-fiberized LAGP continuous skeleton. Sci. China Mater. (2024).https://doi.org/10.1007/s40843-024-3104-2
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