Abstract

Pyrite FeS2 now emerges as a promising anode for potassium-ion batteries (PIBs) due to its low cost and high theoretical capacity. However, the significant volume expansion, low electrical conductivity, and the ambiguous mechanism related to potassium storage severely hinder its development for PIBs anodes. Herein, FeS2 nanostructures are skillfully dispersed on the graphene surface layer by layer (FeS2@C-rGO) to form a sandwich structure by using Fe-based metal organic framework (Fe-MOF) as precursors. The unique structural design can improve the transfer kinetics of K+ and effectively buffer the volume expansion during cycling, thereby enhancing the potassium storage performance. As a result, the FeS2@C-rGO delivers a high capacity of 550 mAh/g at a current density of 0.1 A/g. At a high rate of 2 A/g, the capacity can maintain 171 mAh/g even after 500 cycles. Moreover, the electrochemical reaction mechanism and potassium storage behavior are revealed by in-situ X-ray diffractionand density functional theory calculations. This work not only provides a novel insight into the structural design of electrode materials for high-performance PIBs, but also proposes a valuable understanding of the potassium storage mechanism of the FeS2-based anode.

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