Nature Energy ( IF 49.7 ) Pub Date : 2024-07-31 , DOI: 10.1038/s41560-024-01596-6 Longfei Cui , Shu Zhang , Jiangwei Ju , Tao Liu , Yue Zheng , Jiahao Xu , Yantao Wang , Jiedong Li , Jingwen Zhao , Jun Ma , Jinzhi Wang , Gaojie Xu , Ting-Shan Chan , Yu-Cheng Huang , Shu-Chih Haw , Jin-Ming Chen , Zhiwei Hu , Guanglei Cui
All-solid-state lithium batteries typically employ heterogeneous composite cathodes where conductive additives are introduced to improve mixed conduction. These electrochemically inactive additives are not fully compatible with layered oxide cathodes that undergo large volume change, significantly reducing battery energy density and cycle life. Here we propose a cathode homogenization strategy by cold pressing a zero-strain cathode material with efficient mixed conduction throughout the (dis)charge process. Li1.75Ti2(Ge0.25P0.75S3.8Se0.2)3 possesses considerable Li+/electronic conductivity of 0.22/242 mS cm−1 when fully charged, increasing monotonically to 0.66/412 mS cm−1 when fully discharged. It delivers a specific capacity of 250 mAh g−1 and undergoes a 1.2% volume change. Homogeneous cathodes composed of 100% Li1.75Ti2(Ge0.25P0.75S3.8Se0.2)3 enable room-temperature all-solid-state lithium batteries to achieve a cycle life of over 20,000 cycles at 2.5 C with a specific capacity retention of 70% and a high energy density of 390 Wh kg−1 at the cell level at 0.1 C. This cathode homogenization strategy contrasts to the conventional cathode heterogeneous design, potentially improving the viability of all-solid-state lithium batteries for commercial applications.
中文翻译:
实现长循环寿命全固态锂电池的阴极均质化策略
全固态锂电池通常采用异质复合正极,其中引入导电添加剂以改善混合导电。这些电化学惰性添加剂与经历较大体积变化的层状氧化物正极不完全兼容,从而显着降低电池能量密度和循环寿命。在这里,我们提出了一种阴极均质化策略,通过冷压零应变阴极材料,在整个充电(放电)过程中实现高效的混合传导。 Li 1.75 Ti 2 (Ge 0.25 P 0.75 S 3.8 Se 0.2 ) 3具有相当大的Li + /电子电导率,当完全充电时为0.22/242 mS cm - 1 ,当完全放电时单调增加至0.66/412 mS cm - 1 。它的比容量为250 mAh g -1 ,体积变化为1.2%。由100% Li 1.75 Ti 2 (Ge 0.25 P 0.75 S 3.8 Se 0.2 ) 3组成的均质正极使室温全固态锂电池能够在2.5 C下实现超过20,000次循环的循环寿命,比容量保持率为0.1 C 下电池水平的能量密度为 70%,能量密度为 390 Wh kg - 1。这种阴极均质化策略与传统的阴极异质设计形成鲜明对比,有可能提高全固态锂电池在商业应用中的可行性。