Liu Mingwei, Wan Lei, Su Pei, Guo Taotao, Yin Ruojiao, Jin Haize, Jia Henan, Tang Fuling
School of Materials Science and Engineering, Lanzhou University of Technology, Lanzhou 730050, People's Republic of China; State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals, Lanzhou University of Technology, Lanzhou 730050, People's Republic of China.
School of Materials Science and Engineering, Lanzhou University of Technology, Lanzhou 730050, People's Republic of China; State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals, Lanzhou University of Technology, Lanzhou 730050, People's Republic of China.
J Colloid Interface Sci. 2025 Mar 15;682:436-445. doi: 10.1016/j.jcis.2024.11.211. Epub 2024 Dec 1.
The shuttle effect of lithium polysulfides (LiPSs) and sluggish sulfur conversion kinetics have seriously hindered the commercial application of lithium-sulfur (Li-S) batteries. Currently, the adsorption and catalysis processes are emphasized; however, the diffusion process is often neglected. The delayed diffusion of the adsorbed LiPSs significantly reduce battery performance. Herein, the directional migration of S was realized by adjusting the characteristics of heterostructure materials. The heterostructure consists of Co with a high Fermi level and excellent catalytic activity and CoO with a low Fermi level and strong adsorption ability. This configuration regulated the direction of the built-in electric field (BIEF) at the heterogeneous interface, which promoted the migration of S from CoO to Co side and realised a continuous "adsorption-directional migration-catalysis" mechanism. Experimental and theoretical results indicated that the Co/CoO heterostructure modified by nitrogen-doped carbon nanotubes (Co/CoO@NC-CNTs), as the separator of Li-S batteries, not only enhanced the adsorption of LiPSs but also accelerated the kinetic conversion process. Consequently, the battery modified by the Co/CoO@NC-CNTs separator exhibited a high initial specific capacity of 1423 mAh g at 0.2C, and maintained 735.5 mAh g at a current density of 1C after 400 cycles.
多硫化锂(LiPSs)的穿梭效应和缓慢的硫转化动力学严重阻碍了锂硫(Li-S)电池的商业应用。目前,人们主要关注吸附和催化过程;然而,扩散过程却常常被忽视。被吸附的LiPSs扩散延迟会显著降低电池性能。在此,通过调节异质结构材料的特性实现了硫的定向迁移。该异质结构由具有高费米能级和优异催化活性的钴以及具有低费米能级和强吸附能力的氧化钴组成。这种结构调节了异质界面处内建电场(BIEF)的方向,促进了硫从氧化钴向钴一侧的迁移,并实现了连续的“吸附-定向迁移-催化”机制。实验和理论结果表明,氮掺杂碳纳米管修饰的Co/CoO异质结构(Co/CoO@NC-CNTs)作为Li-S电池的隔膜,不仅增强了对LiPSs的吸附,还加速了动力学转化过程。因此,采用Co/CoO@NC-CNTs隔膜修饰的电池在0.2C时表现出1423 mAh g的高初始比容量,在1C电流密度下循环400次后仍保持735.5 mAh g。