Du Xuan, Ma Dan, Zhang Yuefeng, Ma Jianmin, Wang Jianyi, Xiao Qinggui, Wang Bin, Tian Liangliang, Zhuang Jinliang
National Engineering Research Center of Green Recycling for Strategic Metal Resources, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
CRRC Zhuzhou Locomotive Co., Ltd., No. 1 Tianxin Road, Shifeng District, Zhuzhou City 412000, Hunan Province, China.
Inorg Chem. 2023 Apr 3;62(13):5134-5144. doi: 10.1021/acs.inorgchem.2c04417. Epub 2023 Mar 23.
Despite great achievements having been made in lithium-sulfur batteries (LSBs), further improvements regarding rate performance, cycle life, and operating temperature are needed for realistic applications. Herein, we developed a simple electrospun method for the preparation of TiO coaxial nanofiber (TCNFs)-modified Celgard separators to suppress the polysulfide shuttling. LSBs with a TCNF/Celgard separator display excellent electrochemical performance. For an areal sulfur loading of 2.5 mg cm, the cells exhibited a capacity of 1279 mA h g at 0.5 A g, remained 798 mA h g at 2.5 A g, and low-capacity decay of 0.057% per cycle within 1000 cycles. At 50 and -10 °C, the capacity of the cells is maintained at 932 and 931 mA h g after 80 cycles at 0.5 A g, respectively. Detailed structural analysis and theoretical calculations revealed that the hollow-structured TCNFs offer high density of accessible electropositive Ti sites and oxygen vacancies and thus enables efficient trapping of polysulfides and facilitates Li transfer, leading to excellent performance. The simplicity of this strategy and the diversity of hollow-structured metal oxides holds great promise to design separators for high-performance LSBs.
尽管锂硫电池(LSBs)已取得了巨大成就,但在实际应用中,仍需要在倍率性能、循环寿命和工作温度方面进一步改进。在此,我们开发了一种简单的静电纺丝方法来制备TiO同轴纳米纤维(TCNFs)改性的Celgard隔膜,以抑制多硫化物穿梭。具有TCNF/Celgard隔膜的锂硫电池表现出优异的电化学性能。对于面硫负载量为2.5 mg cm的情况,电池在0.5 A g下的容量为1279 mA h g,在2.5 A g下保持798 mA h g,并且在1000次循环内每循环的低容量衰减为0.057%。在50和-10°C下,电池在0.5 A g下循环80次后,容量分别保持在932和931 mA h g。详细的结构分析和理论计算表明,中空结构的TCNFs提供了高密度的可及正电Ti位点和氧空位,从而能够有效捕获多硫化物并促进Li转移,从而带来优异的性能。这种策略的简单性和中空结构金属氧化物的多样性为设计高性能锂硫电池的隔膜带来了巨大希望。