Dynamic Multistage Coupling of FeS<sub>2</sub>/S Enables Ultrahigh Reversible Na–S Batteries

Authors: Cunshuang Ma, Xiang Wang, Jiaqi Lan, Jiyu Zhang, Keming Song, Jiacheng Chen, Junmin Ge, Weihua Chen

Published: 2022-11-20

DOI: 10.1002/adfm.202211821

Source: Full article


Abstract

AbstractThe fundamental challenges that coexisted around sulfur cathode energy storage systems, are the severe polysulfide dissolution and low reactivity resulting in poor reversibility and short cycle life, specifically, in inexpensive sodium ion batteries. Herein, the solution‐processed synthesis of ultra‐high intimate contacted FeS2/S architecture is reported and evolution of the dynamic multistage coupling between the FeS2 and S in sodium–sulfur batteries is revealed. Atomic visualization and in situ spectroscopy conclude that: NaxFeS2 (0 <x ≤1) effectively captures sodium polysulfides and promotes the conversion of S8 to Na2S4 to Na2S2/Na2S; simultaneously, the presence of Na2S2/Na2S traps the continuous growth of iron grains during continuously discharging to 0.4 V, thereby boosting the reversibility and high capacity. Moreover, the density functional theory further analyses the unique coupling effect of Na2Sx with different intermediate states of FeS2. The electrode with unique structure and dynamic coupling exhibits outstanding cycle reversibility and extremely long life, which delivers a reversible capacity of 860 mAh g−1 after 1000 cycles with no capacity decay at 0.5 A g−1. Even under a practical areal capacity of 4 mAh cm−2, it still shows pretty‐well cycling stability.