School of Material Science and Engineering & Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Wuhan Institute of Technology, Wuhan, 430205, China.
School of Resource and Environmental Sciences, Wuhan University, Wuhan, 430072, China.
Adv Sci (Weinh). 2022 Dec;9(35):e2204561. doi: 10.1002/advs.202204561. Epub 2022 Oct 26.
The shuttle effect of lithium polysulfides in lithium-sulfur batteries (LSBs) has a detrimental impact on their electrochemical performance. To effectively mitigate the shuttle effect, in this study, the coral-like CuS is introduced to modify the carbon nanotube (CNTs), which is coated on commercial separator and served as the S cathode interlayer (PE@CuS/CNTs). The CuS/CNTs interlayer possesses efficient physical impediment and chemisorption to polysulfide anions. When achieving maximum adsorption to polysulfide anions, a "polysulfide-phobic" surface would be formed as a shield to restrain the polysulfide anions in the cathode region. Simultaneously, the CuS/CNTs interlayer can improve the lithium ion diffusion and guarantee desirable electrochemical reaction kinetics. Consequently, the LSBs with PE@CuS/CNTs show an initial discharge capacity of 1242.4 mAh g at 0.5 C (1 C = 1675 mA g ) and retain a long-term cycling stability (568.5 mAh g after 1000 cycles, 2 C), corresponding to an ultra-low capacity fading rate of only 0.05% per cycle. Also, the LSBs with PE@CuS/CNTs exhibit high resistance to self-discharge and favorable performance under high S loading (4.5 mg cm ) and lean electrolyte (9.4 mL g ).
锂硫电池(LSB)中多硫化物的穿梭效应对其电化学性能有不利影响。为了有效抑制穿梭效应,本研究引入珊瑚状的 CuS 对碳纳米管(CNTs)进行修饰,将其涂覆在商业隔膜上作为 S 正极中间层(PE@CuS/CNTs)。CuS/CNTs 中间层对多硫化物阴离子具有有效的物理阻碍和化学吸附作用。当达到对多硫化物阴离子的最大吸附时,会形成一个“排斥多硫化物”的表面作为屏蔽层,将多硫化物阴离子限制在正极区域内。同时,CuS/CNTs 中间层可以提高锂离子的扩散能力,并保证理想的电化学反应动力学。因此,具有 PE@CuS/CNTs 的 LSB 在 0.5 C(1 C = 1675 mA g )时的初始放电容量为 1242.4 mAh g ,并具有长期循环稳定性(1000 次循环后为 568.5 mAh g ,2 C),对应的容量衰减率仅为 0.05%/循环。此外,具有 PE@CuS/CNTs 的 LSB 具有很高的抗自放电能力,在高 S 负载(4.5 mg cm )和贫电解液(9.4 mL g )下也表现出良好的性能。