Sulfur–Carbon Electrode with PEO‐LiFSI‐PVDF Composite Coating for High‐Rate and Long‐Life Lithium–Sulfur Batteries

作者：Ling Li, Jong Seok Nam, Min Soo Kim, Yifan Wang, Shaohua Jiang, Haoqing Hou, Il‐Doo Kim · 发表于：Advanced Energy Materials · 年份：2023 · DOI：10.1002/aenm.202302139 · 被引用次数：126 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Flame retardant materials and properties

Abstract To address the problem of the serious capacity fading in lithium–sulfur batteries, a multi‐functional PEO(polyethylene oxide)/LiFSI (lithium bis(fluorosulfonyl)imide)/PVDF (polyvinylidene fluoride) (PLP) gel polymer electrolyte is exploited by coating PLP on a carbon nanotubes (CNTs) based sulfur cathode (PLP‐S/CNTs) with a controlled thermal annealing process. The annealing process leads to the conformal infusion of PLP through the matrix of S/CNTs with retaining the amorphous phase of the PLP, which enhance the rate performance compared to the bare S/CNTs. The PLP coating drives the transformation of more elemental sulfur to Li 2 S 2 /Li 2 S without forming intermediary product by restraining soluble‐polysulfides formation. Furthermore, the PLP coating successfully inhibits the dissolution of Li 2 S x ( x > 4) in PEO and prevents the loss of active material in the cathode, which is confirmed by density functional theory calculations. Comprehensively, the PLP coating applied to the surface of the S/CNTs cathode exhibit significantly suppressed shuttle effect and greatly improve long‐term cycle stability of the lithium–sulfur battery. The synthesized PLP‐coated S/CNTs composite cathode demonstrates a high specific capacity of 573.6 mAh g −1 at a current density of 0.5 C after 1 000 cycles, even achieving 318.1 mAh g −1 at an extremely high C‐rate (6 C). which is unprecedented performance among the reported studies on coating technology.