Zheng Yun, Yang Na, Gao Rui, Li Zhaoqiang, Dou Haozhen, Li Gaoran, Qian Lanting, Deng Yaping, Liang Jiequan, Yang Leixin, Liu Yizhou, Ma Qianyi, Luo Dan, Zhu Ning, Li Kecheng, Wang Xin, Chen Zhongwei
Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1, Canada.
South China Academy of Advanced Optoelectronics, School of Information and Optoelectronic Science and Engineering, International Academy of Optoelectronics at Zhaoqing, South China Normal University, Guangzhou, 510006, China.
Adv Mater. 2022 Nov;34(44):e2203417. doi: 10.1002/adma.202203417. Epub 2022 Oct 3.
The construction of robust (quasi)-solid-state electrolyte (SSE) for flexible lithium-metal batteries is desirable but extremely challenging. Herein, a novel, flexible, and robust quasi-solid-state electrolyte (QSSE) with a "tree-trunk" design is reported for ultralong-life lithium-metal batteries (LMBs). An in-situ-grown metal-organic framework (MOF) layer covers the cellulose-based framework to form hierarchical ion-channels, enabling rapid ionic transfer kinetics and excellent durability. A conductivity of 1.36 × 10 S cm , a transference number of 0.72, an electrochemical window of 5.26 V, and a good rate performance are achieved. The flexible LMBs fabricated with as-designed QSSEs deliver areal capacity of up to 3.1 mAh cm at the initial cycle with high mass loading of 14.8 mg cm in Li-NCM811 cells and can retain ≈80% capacity retention after 300 cycles. An ultralong-life of 3000 cycles (6000 h) is also achieved in Li-LiFePO cells. This work presents a promising route in constructing a flexible QSSE toward ultralong-life LMBs, and also provides a design rationale for material and structure development in the area of energy storage and conversion.
构建用于柔性锂金属电池的坚固（准）固态电解质（SSE）是理想的，但极具挑战性。在此，报道了一种具有“树干”设计的新型、柔性且坚固的准固态电解质（QSSE），用于超长寿命锂金属电池（LMB）。原位生长的金属有机框架（MOF）层覆盖在纤维素基框架上，形成分级离子通道，实现快速的离子转移动力学和出色的耐久性。实现了1.36×10⁻³ S cm⁻¹的电导率、0.72的迁移数、5.26 V的电化学窗口以及良好的倍率性能。用设计的QSSE制造的柔性LMB在Li-NCM811电池中，初始循环时在14.8 mg cm⁻²的高质量负载下可提供高达3.1 mAh cm⁻²的面积容量，并且在300次循环后可保持约80%的容量保持率。在Li-LiFePO₄电池中也实现了3000次循环（6000小时）的超长寿命。这项工作为构建用于超长寿命LMBs的柔性QSSE提供了一条有前景的途径，也为储能和转换领域的材料和结构开发提供了设计原理。
