Li Zhong, Pan Qiyun, Yang Peiyue, Jiang Shan, Zheng Zhongxiang, Wu Wenfei, Xia Jingyi, Tang Sishi, Wu Dabei, Cao Yi, Xuan Jinnan, Yang Lun, Ma Longlong, Tian Yayang
Institute for Advanced Materials, Hubei Normal University, 435002, Huangshi, China.
Department of Chemistry, Changzhi University, 046011, Changzhi, China.
Chemistry. 2023 Nov 13;29(63):e202302334. doi: 10.1002/chem.202302334. Epub 2023 Oct 4.
Lithium-sulfur batteries are believed to possess the feasibility to power electric vehicles in the future ascribed to the competitive energy density. However, soluble polysulfides continuously shuttle between the sulfur electrode and lithium anode across the separator, which dramatically impairs the battery's capacity. Herein, the surface of a polypropylene separator (PP film) is successfully modified with a delicately designed cation-selective polymer layer to suppress the transport of polysulfides. In principle, since bis-sulfonimide anions groups on the backbone of the polymer are immobilized, only cations can pass through the polymer layer. Furthermore, plenty of ethoxy chains in the polymer can facilitate lithium-ion mobility. Consequently, in addition to obstructing the movement of negatively charged polysulfides by the electrostatic repulsive force of fixed anions, the coated multi-functional layer on the PP film also guarantees the smooth conduction of lithium ions. The investigations demonstrate that the battery with the pristine PP film only delivers 228.5 mAh g after 300 cycles at 2 C with a high capacity fading rate of 60.9 %. By contrast, the polymer-coated sample can release 409.4 mAh g under the identical test condition and the capacity fading rate sharply declines to 43.2 %, illustrating superior cycle performance.
锂硫电池因其具有竞争力的能量密度,被认为在未来具备为电动汽车供电的可行性。然而,可溶性多硫化物会持续在硫电极和锂阳极之间穿过隔膜穿梭,这极大地损害了电池的容量。在此,通过精心设计的阳离子选择性聚合物层成功修饰了聚丙烯隔膜(PP膜)的表面,以抑制多硫化物的传输。原则上,由于聚合物主链上的双磺酰亚胺阴离子基团被固定,只有阳离子能够穿过聚合物层。此外,聚合物中大量的乙氧基链可以促进锂离子的迁移。因此,PP膜上涂覆的多功能层除了通过固定阴离子的静电排斥力阻碍带负电的多硫化物的移动外,还保证了锂离子的顺畅传导。研究表明,仅使用原始PP膜的电池在2C下经过300次循环后,仅能提供228.5 mAh g的电量,容量衰减率高达60.9%。相比之下,聚合物涂覆的样品在相同测试条件下可释放409.4 mAh g的电量,容量衰减率急剧下降至43.2%,显示出优异的循环性能。