Nature Communications ( IF 14.7 ) Pub Date : 2022-06-09 , DOI: 10.1038/s41467-022-30788-5 Zongjie Sun 1 , Kai Xi 1 , Jing Chen 1 , Amor Abdelkader 2 , Meng-Yang Li 1 , Yuanyuan Qin 1 , Yue Lin 3 , Qiu Jiang 4 , Ya-Qiong Su 1 , R Vasant Kumar 5 , Shujiang Ding 1
Ionic-conductive polymers are appealing electrolyte materials for solid-state lithium-based batteries. However, these polymers are detrimentally affected by the electrochemically-inactive anion migration that limits the ionic conductivity and accelerates cell failure. To circumvent this issue, we propose the use of polyvinyl ferrocene (PVF) as positive electrode active material. The PVF acts as an anion-acceptor during redox processes, thus simultaneously setting anions and lithium ions as effective charge carriers. We report the testing of various Li||PVF lab-scale cells using polyethylene oxide (PEO) matrix and Li-containing salts with different anions. Interestingly, the cells using the PEO-lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) solid electrolyte deliver an initial capacity of 108 mAh g−1 at 100 μA cm−2 and 60 °C, and a discharge capacity retention of 70% (i.e., 70 mAh g−1) after 2800 cycles at 300 μA cm−2 and 60 °C. The Li|PEO-LiTFSI|PVF cells tested at 50 μA cm−2 and 30 °C can also deliver an initial discharge capacity of around 98 mAh g−1 with an electrolyte ionic conductivity in the order of 10−5 S cm−1.
中文翻译:
使用负离子阴极扩展锂基电池中聚合物电解质的活性电荷载体
离子导电聚合物是用于固态锂基电池的有吸引力的电解质材料。然而,这些聚合物受到电化学惰性阴离子迁移的不利影响,这种迁移限制了离子电导率并加速了电池故障。为了避免这个问题,我们建议使用聚乙烯二茂铁(PVF)作为正极活性材料。PVF 在氧化还原过程中充当阴离子受体,因此同时将阴离子和锂离子设置为有效的电荷载体。我们报告了使用聚环氧乙烷 (PEO) 基质和具有不同阴离子的含锂盐对各种 Li||PVF 实验室规模电池的测试。有趣的是,使用 PEO-锂双(三氟甲磺酰基)亚胺 (LiTFSI) 固体电解质的电池可提供 108 mAh g −1的初始容量在 100 μA cm -2和 60 °C 下,在 300 μA cm -2和 60 °C 下经过 2800 次循环后,放电容量保持率为 70%(即 70 mAh g -1 )。在 50 μA cm -2和 30 °C 下测试的 Li|PEO-LiTFSI|PVF 电池还可以提供约 98 mAh g -1的初始放电容量,电解质离子电导率约为 10 -5 S cm -1 .